Pressure-Tuneable Visible-Range Band Gap in the Ionic Spinel Tin Nitride

John S.C. Kearney; Miglė Graužinytė; Dean Smith; Daniel Sneed; Christian Childs; Jasmine Hinton; Changyong Park; Jesse S. Smith; Eunja Kim; Samuel D.S. Fitch; Andrew L. Hector; Chris J. Pickard; José A. Flores-Livas; Ashkan Salamat

doi:10.1002/anie.201805038

Pressure-Tuneable Visible-Range Band Gap in the Ionic Spinel Tin Nitride

John S.C. Kearney
, Miglė Graužinytė
, Dean Smith
, Daniel Sneed
, Christian Childs
, Jasmine Hinton
, Changyong Park
, Jesse S. Smith
, Eunja Kim
, Samuel D.S. Fitch
, Andrew L. Hector
, Chris J. Pickard
, José A. Flores-Livas
, Ashkan Salamat

Research output: Contribution to journal › Article › peer-review

27 Scopus citations

Abstract

The application of pressure allows systematic tuning of the charge density of a material cleanly, that is, without changes to the chemical composition via dopants, and exploratory high-pressure experiments can inform the design of bulk syntheses of materials that benefit from their properties under compression. The electronic and structural response of semiconducting tin nitride Sn₃N₄ under compression is now reported. A continuous opening of the optical band gap was observed from 1.3 eV to 3.0 eV over a range of 100 GPa, a 540 nm blue-shift spanning the entire visible spectrum. The pressure-mediated band gap opening is general to this material across numerous high-density polymorphs, implicating the predominant ionic bonding in the material as the cause. The rate of decompression to ambient conditions permits access to recoverable metastable states with varying band gaps energies, opening the possibility of pressure-tuneable electronic properties for future applications.

Original language	English
Pages (from-to)	11623-11628
Number of pages	6
Journal	Angewandte Chemie - International Edition
Volume	57
Issue number	36
DOIs	https://doi.org/10.1002/anie.201805038
State	Published - Sep 3 2018
Externally published	Yes

Funding

We thank Roald Hoffman and Philippe F. Weck for useful discussions. This research was sponsored in part by the National Nuclear Security Administration under the Stewardship Science Academic Alliances program through DOE Cooperative Agreement no. DE-NA0001982. Portions of this work were performed at HPCAT (Sector 16), Advanced Photon Source (APS), Argonne National Laboratory. C.P. and J.S.S. acknowledge the support of DOE-BES/DMSE under Award DE-FG02-99ER45775. HPCAT operation is supported by DOE-NNSA under Award No. DE-NA0001974, with partial instrumentation funding by NSF. C.J.P. acknowledges financial support from the Engineering and Physical Sciences Research Council (EPSRC) of the UK under Grant No. EP/P022596/1. C.J.P. is also supported by the Royal Society through a Royal Society Wolfson Research Merit Award. J.A.F.-L. acknowledges fruitful discussions with Andris Gulans on the GW-LAPW calculations as well as substantial computational resources under the project (s752) from the Swiss National Supercomputing Center (CSCS) in Lugano. This research was partially supported by the NCCR MARVEL, funded by the SWISS National Science Foundation.

Keywords

ab initio calculations
high-pressure chemistry
nitrides
semiconductors

Access to Document

10.1002/anie.201805038

Cite this

Kearney, J. S. C., Graužinytė, M., Smith, D., Sneed, D., Childs, C., Hinton, J., Park, C., Smith, J. S., Kim, E., Fitch, S. D. S., Hector, A. L., Pickard, C. J., Flores-Livas, J. A., & Salamat, A. (2018). Pressure-Tuneable Visible-Range Band Gap in the Ionic Spinel Tin Nitride. Angewandte Chemie - International Edition, 57(36), 11623-11628. https://doi.org/10.1002/anie.201805038

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AU - Smith, Jesse S.

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AU - Hector, Andrew L.

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AB - The application of pressure allows systematic tuning of the charge density of a material cleanly, that is, without changes to the chemical composition via dopants, and exploratory high-pressure experiments can inform the design of bulk syntheses of materials that benefit from their properties under compression. The electronic and structural response of semiconducting tin nitride Sn3N4 under compression is now reported. A continuous opening of the optical band gap was observed from 1.3 eV to 3.0 eV over a range of 100 GPa, a 540 nm blue-shift spanning the entire visible spectrum. The pressure-mediated band gap opening is general to this material across numerous high-density polymorphs, implicating the predominant ionic bonding in the material as the cause. The rate of decompression to ambient conditions permits access to recoverable metastable states with varying band gaps energies, opening the possibility of pressure-tuneable electronic properties for future applications.

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Pressure-Tuneable Visible-Range Band Gap in the Ionic Spinel Tin Nitride

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