Heterovalent Dopant Incorporation for Bandgap and Type Engineering of Perovskite Crystals

Ahmed L. Abdelhady; Makhsud I. Saidaminov; Murali Banavoth; Valerio Adinolfi; Oleksandr Voznyy; Khabiboulakh Katsiev; Erkki Alarousu; Riccardo Comin; Ibrahim Dursun; Lutfan Sinatra; Edward H. Sargent; Omar F. Mohammed; Osman Bakr

doi:10.1021/acs.jpclett.5b02681

Heterovalent Dopant Incorporation for Bandgap and Type Engineering of Perovskite Crystals

Ahmed L. Abdelhady, Makhsud I. Saidaminov, Murali Banavoth, Valerio Adinolfi, Oleksandr Voznyy, Khabiboulakh Katsiev, Erkki Alarousu, Riccardo Comin, Ibrahim Dursun, Lutfan Sinatra, Edward H. Sargent, Omar F. Mohammed, Osman Bakr

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340 Scopus citations

Abstract

Controllable doping of semiconductors is a fundamental technological requirement for electronic and optoelectronic devices. As intrinsic semiconductors, hybrid perovskites have so far been a phenomenal success in photovoltaics. The inability to dope these materials heterovalently (or aliovalently) has greatly limited their wider utilizations in electronics. Here we show an efficient in situ chemical route that achieves the controlled incorporation of trivalent cations (Bi3+, Au3+, or In3+) by exploiting the retrograde solubility behavior of perovskites. We term the new method dopant incorporation in the retrograde regime. We achieve Bi3+ incorporation that leads to bandgap tuning (∼300 meV), 104 fold enhancement in electrical conductivity, and a change in the sign of majority charge carriers from positive to negative. This work demonstrates the successful incorporation of dopants into perovskite crystals while preserving the host lattice structure, opening new avenues to tailor the electronic and optoelectronic properties of this rapidly emerging class of solution-processed semiconductors. © 2016 American Chemical Society.

Original language	English (US)
Pages (from-to)	295-301
Number of pages	7
Journal	The Journal of Physical Chemistry Letters
Volume	7
Issue number	2
DOIs	https://doi.org/10.1021/acs.jpclett.5b02681
State	Published - Jan 7 2016

Bibliographical note

KAUST Repository Item: Exported on 2020-10-01
Acknowledged KAUST grant number(s): URF/1/1373-01-01, URF/1/1741-01-01, URF/1/2268-01-01
Acknowledgements: The authors acknowledge the support of Awards URF/1/2268-01-01, URF/1/1741-01-01, and URF/1/1373-01-01 made by King Abdullah University of Science and Technology (KAUST). We acknowledge the financial support from King Abdulaziz City for Science and Technology (KACST), Grant KACST TIC R2-FP-008. The authors thank Y. Losovyj for XPS date collection and partial analysis, and P. Dowben for the useful discussions. Access to XPS at the Nanoscience Characterization Facility of Indiana University's Nanoscience Center was provided by the NSF (Award DMR MRI-1126394).

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10.1021/acs.jpclett.5b02681

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Abdelhady, A. L., Saidaminov, M. I., Banavoth, M., Adinolfi, V., Voznyy, O., Katsiev, K., Alarousu, E., Comin, R., Dursun, I., Sinatra, L., Sargent, E. H., Mohammed, O. F., & Bakr, O. (2016). Heterovalent Dopant Incorporation for Bandgap and Type Engineering of Perovskite Crystals. The Journal of Physical Chemistry Letters, 7(2), 295-301. https://doi.org/10.1021/acs.jpclett.5b02681

@article{a04e14902b4a4d7e93cb6dba7254de25,

title = "Heterovalent Dopant Incorporation for Bandgap and Type Engineering of Perovskite Crystals",

abstract = "Controllable doping of semiconductors is a fundamental technological requirement for electronic and optoelectronic devices. As intrinsic semiconductors, hybrid perovskites have so far been a phenomenal success in photovoltaics. The inability to dope these materials heterovalently (or aliovalently) has greatly limited their wider utilizations in electronics. Here we show an efficient in situ chemical route that achieves the controlled incorporation of trivalent cations (Bi3+, Au3+, or In3+) by exploiting the retrograde solubility behavior of perovskites. We term the new method dopant incorporation in the retrograde regime. We achieve Bi3+ incorporation that leads to bandgap tuning (∼300 meV), 104 fold enhancement in electrical conductivity, and a change in the sign of majority charge carriers from positive to negative. This work demonstrates the successful incorporation of dopants into perovskite crystals while preserving the host lattice structure, opening new avenues to tailor the electronic and optoelectronic properties of this rapidly emerging class of solution-processed semiconductors. {\textcopyright} 2016 American Chemical Society.",

author = "Abdelhady, {Ahmed L.} and Saidaminov, {Makhsud I.} and Murali Banavoth and Valerio Adinolfi and Oleksandr Voznyy and Khabiboulakh Katsiev and Erkki Alarousu and Riccardo Comin and Ibrahim Dursun and Lutfan Sinatra and Sargent, {Edward H.} and Mohammed, {Omar F.} and Osman Bakr",

note = "KAUST Repository Item: Exported on 2020-10-01 Acknowledged KAUST grant number(s): URF/1/1373-01-01, URF/1/1741-01-01, URF/1/2268-01-01 Acknowledgements: The authors acknowledge the support of Awards URF/1/2268-01-01, URF/1/1741-01-01, and URF/1/1373-01-01 made by King Abdullah University of Science and Technology (KAUST). We acknowledge the financial support from King Abdulaziz City for Science and Technology (KACST), Grant KACST TIC R2-FP-008. The authors thank Y. Losovyj for XPS date collection and partial analysis, and P. Dowben for the useful discussions. Access to XPS at the Nanoscience Characterization Facility of Indiana University's Nanoscience Center was provided by the NSF (Award DMR MRI-1126394).",

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month = jan,

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doi = "10.1021/acs.jpclett.5b02681",

language = "English (US)",

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Abdelhady, AL, Saidaminov, MI, Banavoth, M, Adinolfi, V, Voznyy, O, Katsiev, K, Alarousu, E, Comin, R, Dursun, I, Sinatra, L, Sargent, EH, Mohammed, OF & Bakr, O 2016, 'Heterovalent Dopant Incorporation for Bandgap and Type Engineering of Perovskite Crystals', The Journal of Physical Chemistry Letters, vol. 7, no. 2, pp. 295-301. https://doi.org/10.1021/acs.jpclett.5b02681

TY - JOUR

T1 - Heterovalent Dopant Incorporation for Bandgap and Type Engineering of Perovskite Crystals

AU - Abdelhady, Ahmed L.

AU - Saidaminov, Makhsud I.

AU - Banavoth, Murali

AU - Adinolfi, Valerio

AU - Voznyy, Oleksandr

AU - Katsiev, Khabiboulakh

AU - Alarousu, Erkki

AU - Comin, Riccardo

AU - Dursun, Ibrahim

AU - Sinatra, Lutfan

AU - Sargent, Edward H.

AU - Mohammed, Omar F.

AU - Bakr, Osman

N1 - KAUST Repository Item: Exported on 2020-10-01 Acknowledged KAUST grant number(s): URF/1/1373-01-01, URF/1/1741-01-01, URF/1/2268-01-01 Acknowledgements: The authors acknowledge the support of Awards URF/1/2268-01-01, URF/1/1741-01-01, and URF/1/1373-01-01 made by King Abdullah University of Science and Technology (KAUST). We acknowledge the financial support from King Abdulaziz City for Science and Technology (KACST), Grant KACST TIC R2-FP-008. The authors thank Y. Losovyj for XPS date collection and partial analysis, and P. Dowben for the useful discussions. Access to XPS at the Nanoscience Characterization Facility of Indiana University's Nanoscience Center was provided by the NSF (Award DMR MRI-1126394).

PY - 2016/1/7

Y1 - 2016/1/7

N2 - Controllable doping of semiconductors is a fundamental technological requirement for electronic and optoelectronic devices. As intrinsic semiconductors, hybrid perovskites have so far been a phenomenal success in photovoltaics. The inability to dope these materials heterovalently (or aliovalently) has greatly limited their wider utilizations in electronics. Here we show an efficient in situ chemical route that achieves the controlled incorporation of trivalent cations (Bi3+, Au3+, or In3+) by exploiting the retrograde solubility behavior of perovskites. We term the new method dopant incorporation in the retrograde regime. We achieve Bi3+ incorporation that leads to bandgap tuning (∼300 meV), 104 fold enhancement in electrical conductivity, and a change in the sign of majority charge carriers from positive to negative. This work demonstrates the successful incorporation of dopants into perovskite crystals while preserving the host lattice structure, opening new avenues to tailor the electronic and optoelectronic properties of this rapidly emerging class of solution-processed semiconductors. © 2016 American Chemical Society.

AB - Controllable doping of semiconductors is a fundamental technological requirement for electronic and optoelectronic devices. As intrinsic semiconductors, hybrid perovskites have so far been a phenomenal success in photovoltaics. The inability to dope these materials heterovalently (or aliovalently) has greatly limited their wider utilizations in electronics. Here we show an efficient in situ chemical route that achieves the controlled incorporation of trivalent cations (Bi3+, Au3+, or In3+) by exploiting the retrograde solubility behavior of perovskites. We term the new method dopant incorporation in the retrograde regime. We achieve Bi3+ incorporation that leads to bandgap tuning (∼300 meV), 104 fold enhancement in electrical conductivity, and a change in the sign of majority charge carriers from positive to negative. This work demonstrates the successful incorporation of dopants into perovskite crystals while preserving the host lattice structure, opening new avenues to tailor the electronic and optoelectronic properties of this rapidly emerging class of solution-processed semiconductors. © 2016 American Chemical Society.

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UR - http://pubs.acs.org/doi/abs/10.1021/acs.jpclett.5b02681

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U2 - 10.1021/acs.jpclett.5b02681

DO - 10.1021/acs.jpclett.5b02681

M3 - Article

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SN - 1948-7185

VL - 7

SP - 295

EP - 301

JO - The Journal of Physical Chemistry Letters

JF - The Journal of Physical Chemistry Letters

IS - 2

ER -

Heterovalent Dopant Incorporation for Bandgap and Type Engineering of Perovskite Crystals

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