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@ARTICLE{Songvilay:859544,
author = {Songvilay, M. and Bari, M. and Ye, Z.-G. and Xu, Guangyong
and Gehring, P. M. and Ratcliff, W. D. and Schmalzl, K. and
Bourdarot, F. and Roessli, B. and Stock, C.},
title = {{L}ifetime-shortened acoustic phonons and static order at
the {B}rillouin zone boundary in the organic-inorganic
perovskite {CH} 3 {NH} 3 {P}b{C}l 3},
journal = {Physical review materials},
volume = {2},
number = {12},
issn = {2475-9953},
address = {College Park, MD},
publisher = {APS},
reportid = {FZJ-2019-00396},
pages = {123601},
year = {2018},
abstract = {Lead halide hybrid perovskites consist of an inorganic
framework hosting a molecular cation located in the
interstitial space. These compounds have been extensively
studied as they have been identified as promising materials
for photovoltaic applications with the interaction between
the molecular cation and the inorganic framework implicated
as influential for the electronic properties. CH3NH3PbCl3
undergoes two structural transitions from a high temperature
cubic unit cell to a tetragonal phase at 177 K and then a
subsequent orthorhombic transition at 170 K. We have
measured the low-frequency lattice dynamics using neutron
spectroscopy and observe an energy broadening in the
acoustic phonon linewidth towards the high-symmetry point
QX=(2,12,0) when approaching the transitions. Concomitant
with these zone boundary anomalies is a hardening of the
entire acoustic phonon branch measured in the q→0 limit
near the (2, 0, 0) Bragg position with decreasing
temperature. Measurements of the elastic scattering at the
Brillouin zone edges QX=(2,12,0),QM=(32,12,0), and
QR=(32,32,52) show Bragg peaks appearing below these
structural transitions. Based on selection rules of neutron
scattering, we suggest that the higher 177 K transition is
displacive with a distortion of the local octahedral
environment and the lower transition is a rigid tilt
transition of the octahedra. We do not observe any critical
broadening in energy or momentum, beyond resolution, of
these peaks near the transitions. We compare these results
to the critical properties reported near the structural
transitions in other perovskites and particularly CsPbCl3
[Y. Fujii, S. Hoshino, Y. Yamada, and G. Shirane, Phys. Rev.
B 9, 4549 (1974)]. We suggest that the simultaneous onset of
static resolution-limited Bragg peaks at the zone boundaries
and the changes in acoustic phonon energies near the zone
center is evidence of a coupling between the inorganic
framework and the molecular cation. The results also
highlight the importance of displacive transitions in
organic-inorganic hybrid perovskites.},
cin = {JCNS-2 / PGI-4 / JARA-FIT / JCNS-ILL},
ddc = {530},
cid = {I:(DE-Juel1)JCNS-2-20110106 / I:(DE-Juel1)PGI-4-20110106 /
$I:(DE-82)080009_20140620$ / I:(DE-Juel1)JCNS-ILL-20110128},
pnm = {144 - Controlling Collective States (POF3-144) / 524 -
Controlling Collective States (POF3-524) / 6212 - Quantum
Condensed Matter: Magnetism, Superconductivity (POF3-621) /
6213 - Materials and Processes for Energy and Transport
Technologies (POF3-621) / 6G4 - Jülich Centre for Neutron
Research (JCNS) (POF3-623)},
pid = {G:(DE-HGF)POF3-144 / G:(DE-HGF)POF3-524 /
G:(DE-HGF)POF3-6212 / G:(DE-HGF)POF3-6213 /
G:(DE-HGF)POF3-6G4},
experiment = {EXP:(DE-Juel1)ILL-IN12-20150421},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000452319500002},
doi = {10.1103/PhysRevMaterials.2.123601},
url = {https://juser.fz-juelich.de/record/859544},
}