Dynamics of Hydride Ions in Metal Hydride-Reduced BaTiO3 Samples Investigated

with Quasielastic Neutron Scattering (Supporting Information)

Carin Eklöf-Österberg,a Reji Nedumkandathil,b Ulrich Häussermann,b Aleksander Jaworski,b Andrew J. Pell,b Madhusudan
Tyagi,c,d Niina H. Jalarvo,e Bernhard Frick, f Antonio Faraone,c and Maths Karlsson,∗,a
a Department of Chemistry and Chemical Engineering, Chalmers University of Technology, SE-412 96 Göteborg, Sweden. E-mail:
maths.karlsson@chalmers.se, Tel: +46 733873207; b Department of Materials and Environmental Chemistry, Stockholm University, SE-10691
Stockholm, Sweden; c NIST Center for Neutron Research, National Institute of Standards and Technology, 100 Bureau Drive, Gaithersburg,
Maryland 20899-6102, United States; d Department of Materials Science and Engineering, University of Maryland, College Park, MD 20742,
United States;e Chemical and Engineering Materials Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831-6475, United
States; f Institut Laue-Langevin, 71, Avenue des Martyrs, Grenoble 38000, France.

1 Structural Characterization Analyses 1.2 Rietveld Refinements of PXRD Patterns

1.1 Photograph of Metal Hydride Reduced BaTiO3

CA1 Experimental data
Fit

Intensity (arb. units)

Difference
Bragg positions

20 30 40 50 60 70 80 90
2θ (°)

CA2 Experimental data

Fit
Intensity (arb. units)

Difference
Bragg positions
Fig. S1 Photograph of a metal hydride reduced BaTiO3 sample. No-
tice the dark blue color, a manifestation of the hydride ion exchange.

20 30 40 50 60 70 80 90
2θ (°)

NAB Experimental data

Fit
Intensity (arb. units)

Difference
Bragg positions

20 30 40 50 60 70 80 90
2θ (°)

Fig. S2 Rietveld fit to the PXRD data of the CA1, CA2, and NAB
samples. The corresponding fit parameters are shown in Table S1.

S1–S4 | S1
1.3 Nuclear Magnetic Resonance Analysis Experimental data T = 400 K T = 500 K
Total fit
Resolution function
L1(Q,ω)
Background

Smeas(Q,ω)
1
BTO H signal integral
CA2 surface H
hydridic H

T = 600 K T = 700 K

Smeas(Q,ω)
BTO CA2

40 20 0 −20 −40 −60

1
H chemical shift [ppm]
ω (μeV) ω (μeV)
Fig. S3 1 H MAS NMR spectra of the precursor material, tetragonal
BaTiO3 (BTO), and the reduced sample CA2 acquired on a 9.4 T Fig. S5 Variable temperature Smeas (Q, ω) of CA2 at Q = 0.9 Å−1 as
spectrometer. The inset shows the proton signal integral with respect measured on BASIS. The spectra have been fitted to function com-
to BTO. prised of an elastic term, a quasielastic component, as described with
a Lorentzian function, and a linear sloping background, as further
explained in the article. The offset of the linear sloping background
background was set to the following values: 0.0005 (400 K), 0.0007
(500 K), 0.0009 (600 K) and 0.0011 (700 K), invariant of Q.
2 Quasielastic Neutron Scattering
2.1 Variable Temperature Quasielastic Spectra Experimental data T = 400 K T = 500 K
Total fit
Resolution function
L1(Q,ω)
Background
Smeas(Q,ω)

Experimental data T = 225 K T = 250 K

Total fit
Resolution function
Smeas(Q,ω)

L1(Q,ω)
Background

T = 600 K T = 700 K
Smeas(Q,ω)

T = 300 K T = 360K
Smeas(Q,ω)

ω (μeV) ω (μeV)

Fig. S6 Variable temperature Smeas (Q, ω) of NAB at Q = 0.9 Å−1 as

ω (μeV)
Fig. S4 Variable temperature Smeas (Q, ω) of CA1 at Q = 1.1 Å−1 as
measured on IN16B. The spectra have been fitted to function com-
prised of an elastic term, a quasielastic component, as described with
a Lorentzian function, and a linear sloping background, as further
explained in the article. Error bars throughout the text represent one
standard deviation.
ω (μeV) measured on BASIS. The spectra have been fitted to function com-
prised of an elastic term, a quasielastic component, as described with
a Lorentzian function, and a linear sloping background, as further ex-
plained in the article. The offset of the linear sloping background was
set to the following values: 0.0012 (400 K), 0.0015 (500 K), 0.0018
(600 K) and 0.0021 (700 K), invariant of Q.

S2 | 1–S4
Table S1 Summary of the Rietveld refinement for the CA1, CA2, and NAB samples.

Sample Lattice parameter (Å) Cell volume (Å3 ) χ2 RBragg RF

CA1 4.0055(2) 64.265(5) 0.859 14.9 11.9
CA2 Phase I: 4.0119(1), 79(2)% 64.580(5) 0.841 2.70 1.97
Phase II: 4.0044(1), 21% 65.43(1)
NAB 4.0044(1) 64.210(1) 0.880 2.09 1.69

S1–S4 | S3
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S4 | 1–S4