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@ARTICLE{Lappas:641876,
author = {Lappas, Alexandros and Kaitatzi, Myrsini and Deltsidis,
Alexandros and Capel Berdiell, Izar and Simonelli, Laura and
Missyul, Alexander and Etter, Martin and Bozin, Emil S.},
title = {{O}rbital-{S}elective {I}nstabilities and {S}pin
{F}luctuations at the {V}erge of {S}uperconductivity in
{I}nterlayer-{E}xpanded {I}ron {S}elenide},
journal = {Chemistry of materials},
volume = {37},
number = {21},
issn = {0897-4756},
address = {Washington, DC},
publisher = {American Chemical Society},
reportid = {PUBDB-2025-05228},
pages = {8581 - 8594},
year = {2025},
abstract = {Understanding electron correlation-driven instabilities and
their coupling to structural phases is essential for
deciphering multiorbital pairing in unconventional
superconductors. We investigate Lix(C5H5N)yFe2Se2 (x ∼
0.6; y ∼ 0.7–0.9), a tetragonal β-FeSe intercalate with
a superconducting transition temperature (Tc = 39 K) closely
tied to an expanded Fe-layer spacing (∼11.4 Å).
High-resolution synchrotron X-ray diffraction and core-level
absorption spectroscopy reveal subtle lattice distortions on
cooling without a symmetry-breaking transition. Instead, the
material exhibits negative thermal expansion (NTE) in the
two-dimensional Fe network below TS ∼ 70 K, and stiffening
of local Se–Fe–Se bond dynamics near Tc. The spatially
incoherent rearrangement of FeSe4 tetrahedra and the
site-local fluctuations, signal reduced electron
correlations compared to those of parent β-FeSe (Tc = 8 K).
Complementary X-ray emission spectroscopy, a fast local
probe of Fe 3d valence states, detects persistent local Fe
spin moments below TS, unlike quenching in related systems.
These findings indicate that decoupling of Fe planes leads
to an electronically driven lattice instability. The latter
emerges as NTE induced from weak, orbital-selective
localization of in-plane Fe 3d states rather than
conventional transverse vibrations. Governed by Hund’s
coupling, this selectivity permits coexistence of local spin
fluctuations with itinerant d-electrons─critical for
enhancing Tc. These results suggest that
intercalation-driven d-orbital differentiation moderates
electron correlations, providing a pathway to optimize the
superconductivity in low-dimensional quantum materials.},
cin = {DOOR ; HAS-User / FS-PET-D},
ddc = {540},
cid = {I:(DE-H253)HAS-User-20120731 /
I:(DE-H253)FS-PET-D-20190712},
pnm = {632 - Materials – Quantum, Complex and Functional
Materials (POF4-632) / 6G3 - PETRA III (DESY) (POF4-6G3)},
pid = {G:(DE-HGF)POF4-632 / G:(DE-HGF)POF4-6G3},
experiment = {EXP:(DE-H253)P-P02.1-20150101},
typ = {PUB:(DE-HGF)16},
doi = {10.1021/acs.chemmater.5c01488},
url = {https://bib-pubdb1.desy.de/record/641876},
}