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@INPROCEEDINGS{Qi:1043681,
author = {Qi, J. and Prakash, P. and Schwärzer, K. and Shahed, H.
and Allgaier, Jürgen and Perßon, J. and Sergeev, I. and
Glazyrin, K. and Rols, S. and De Souza, N. and Yu, D. and
Grzechnik, A. and Angst, M. and Voigt, J. and Friese, K. and
Sohn, Y. and Prajapat, D.},
title = {{E}lucidating entropy contributions of barocaloric effect
in spin crossover complex {F}e({PM}-{B}i{A})2({NCS})2},
reportid = {FZJ-2025-02979},
year = {2025},
abstract = {Background: The barocaloric effect (BCE) is characterized
as a thermal response in solid-state materials induced by
external hydrostatic pressure. Cooling technologies based on
the BCE have emerged as a promising alternative to
conventional vapor-compression cooling. Recently, spin
crossover (SCO) transitions, where the low spin and high
spin states can be switched by hydrostatic pressure, were
proposed as a potential mechanism to generate outstanding
BCE. Fe(PM-BiA)2(NCS)2 (with PM = N-2’- pyridylmethylene
and BiA = 4-aminobiphenyl) is a classic SCO complex that
crystalizes in two different structures, orthorhombic with
abrupt transition and monoclinic with gradual transition. In
this work, we aim to unveil the entropy contributions of
Fe(PM-BiA)2(NCS)2 for optimizing the BCE performance on SCO
complexes. Methods: Spectroscopic methods including nuclear
inelastic scattering (NIS, P01), inelastic neutron
scattering (INS, PANTHER $\&$ PELICAN) and quasi elastic
scattering (QENS, PANTHER $\&$ EMU) have been used for
dynamic studies of Fe(PM-BiA)2(NCS)2. Results: The dynamic
features of both polymorphs over a large energy range are
highlighted by spectroscopic methods. The complete and
Fe-related lattice dynamics have been accessed through INS
and NIS, respectively. It indicates that the Fe-related
entropy change across the spin transition is around $54.6\%$
of the total entropy change. The single crystal X-ray
diffraction evidences the potential dynamic disorder of
phenyl groups. A two-site reorientation mode of the phenyl
group at the ps time scale has been observed by QENS. This
local mode also generates $12\%$ of the total entropy
change.Conclusion: In summary, we confirm that both the
phonon excitations of Fe-N octahedron and the local motions
of phenyl groups play crucial roles in contributing to the
total entropy change in Fe(PM-BiA)2(NCS)2. Our study will
enhance the understanding of the caloric effect in the SCO
complex and promote the application of SCO complexes as BCE
refrigerants.},
month = {Jul},
date = {2025-07-06},
organization = {The International Conference on
Neutron Scattering, Bella Center in
Copenhagen, Denmark, with the last day
at the European Spallation Source (ESS)
in nearby Lund, Sweden (Denmark), 6 Jul
2025 - 10 Jul 2025},
subtyp = {Invited},
cin = {JCNS-2 / JARA-FIT / JCNS-1 / JCNS-4},
cid = {I:(DE-Juel1)JCNS-2-20110106 / $I:(DE-82)080009_20140620$ /
I:(DE-Juel1)JCNS-1-20110106 / I:(DE-Juel1)JCNS-4-20201012},
pnm = {632 - Materials – Quantum, Complex and Functional
Materials (POF4-632) / 6G4 - Jülich Centre for Neutron
Research (JCNS) (FZJ) (POF4-6G4)},
pid = {G:(DE-HGF)POF4-632 / G:(DE-HGF)POF4-6G4},
typ = {PUB:(DE-HGF)24},
url = {https://juser.fz-juelich.de/record/1043681},
}