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New Light-Harvesting Materials Using Accurate
and Effi cient Bandgap Calculations
Ivano E. Castelli ,* Falco Hüser , Mohnish Pandey , Hong Li , Kristian S. Thygesen ,
Brian Seger , Anubhav Jain , Kristin A. Persson , Gerbrand Ceder , and Karsten W. Jacobsen
the search for stable binary and ternary
alloys, 1 batteries, 2 carbon capture and
storage, 3 photovoltaics, 4,5 dye sensitized
solar cells, 6 and water splitting materials
7,8 has been guided by computational
studies. The huge amount of data produced
during these studies has been collected
in several databases, for example,
the Materials Project database, 9 the
AFLOWLIB consortium 1 and the Computational
Materials Repository. 10 , 11
Experimental data are also collected into
databases such as the Inorganic Crystal
Structure Database (ICSD) 12 and the
Landolt-Börnstein database 13 : the former
contains around 160 000 crystal structures,
the latter collects the electronic, magnetic,
thermodynamic properties of 250 000
compounds. The ICSD database is one of
the most complete repositories for crystal
information. Despite this, the electronic
properties are not always available and so
Electronic bandgap calculations are presented for 2400 experimentally known
materials from the Materials Project database and the bandgaps, obtained
with different types of functionals within density functional theory and
(partial) self-consistent GW approximation, are compared for 20 randomly
chosen compounds forming an unconventional set of ternary and quaternary
materials. It is shown that the computationally cheap GLLB-SC potential
gives results in good agreement (around 15%) with the more advanced and
demanding eigenvalue-self-consistent GW. This allows for a high-throughput
screening of materials for different applications where the bandgaps are used
as descriptors for the effi ciency of a photoelectrochemical device. Here, new
light harvesting materials are proposed to be used in a one-photon photoelectrochemical
device for water splitting by combining the estimation of
the bandgaps with the stability analysis using Pourbaix diagrams and with
the evaluation of the position of the band edges. Using this methodology, 25
candidate materials are obtained and 5 of them appear to have a realistic possibility
of being used as photocatalyst in a one-photon water splitting device.
they are not included.
One of the tasks for computational condensed matter scientists
is to fi ll in the missing information in experimental
databases. In this paper, we present the calculations of around
2400 bandgaps of known materials using the GLLB-SC potential
by Gritsenko, van Leeuwen, van Lenthe, and Baerends, 14
(GLLB) adapted by Kuisma et al. 15 to include the correlation
for solids (-SC). The GLLB-SC potential is implemented in the
framework of density functional theory (DFT) in the electronic
structure code GPAW. 16,17 The structures under investigation
are obtained from the Materials Project database. 9 As of March
2014, it contains around 50 000 structures optimized with DFT
from the ICSD entries. We then compare the bandgaps of
20 compounds calculated with different methods, namely local
density approximation (LDA), GLLB-SC, GW approximations
(G 0 W 0 , GW 0 , and GW) and the range-separated hybrid functional
by Heyd, Scuseria, and Ernzerhof (HSE06). At the end,
we apply a screening procedure, discussed in detail and used in
previous works, 7,8 to fi nd new light harvesting materials suitable
for water splitting devices.
2. The Calculation of Bandgaps
Experimental databases mostly contain information about
the crystal structure of materials. It is more complicated to
1. Introduction
High-throughput materials design is becoming more and
more important in materials science thanks to theory developments
that make computer simulations more reliable, and to
an increase in computational resources. During the last decade,
Dr. I. E. Castelli, Dr. F. Hüser, M. Pandey, Dr. H. Li,
Prof. K. S. Thygesen, Prof. K. W. Jacobsen
Center for Atomic-scale Materials Design
Department of Physics
Technical University of Denmark
Kongens Lyngby , DK 2800 , Denmark
E-mail: ivca@fysik.dtu.dk
Dr. B. Seger
Center for Individual Nanoparticle Functionality
Department of Physics
Technical University of Denmark
Kongens Lyngby , DK 2800 , Denmark
Dr. A. Jain, Dr. K. A. Persson
Computational Research Division
Lawrence Berkeley National Laboratory
Berkeley , CA 94720 , USA
Prof. G. Ceder
Massachusetts Institute of Technology
Cambridge , MA 02139 , USA
DOI: 10.1002/aenm.201400915
© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim wileyonlinelibrary.com (1 of 7) 1400915
Adv. Energy Mater. 2015, 5, 1400915
www.advenergymat.de