%0 Journal Article %1 D1TC00785H %A Saito, Yohei %A Rösslhuber, Roland %A Löhle, Anja %A Sanz Alonso, Miriam %A Wenzel, Maxim %A Kawamoto, Atsushi %A Pustogow, Andrej %A Dressel, Martin %D 2021 %I The Royal Society of Chemistry %J J. Mater. Chem. C %K chemical-tuning-molecular-quantum-materials %N 33 %P 10841-10850 %R 10.1039/D1TC00785H %T Chemical tuning of molecular quantum materials κ-(BEDT-TTF)1−x(BEDT-STF)x2Cu2(CN)3: from the Mott-insulating quantum spin liquid to metallic Fermi liquid %U http://dx.doi.org/10.1039/D1TC00785H %V 9 %X The electronic properties of molecular conductors can be readily varied via physical or chemical pressure as it enlarges the bandwidth W. This enables them to cross the Mott insulator-to-metal phase transition by reducing electronic correlations U/W. Here we introduce an alternative path by spatially expanding the molecular orbitals when partially replacing sulfur by selenium in the constituting bis-(ethylenedithio)-tetrathiafulvalene (BEDT-TTF) molecules of the title compound. We characterize how the insulating quantum-spin-liquid state is tuned via a Mott transition to the metallic Fermi-liquid state crossing a narrow region of superconductivity. The transport, dielectric, and optical measurements reveal that at this first-order phase transition, metallic regions coexist in the insulating matrix leading to pronounced percolative effects, which are most obvious in the strong enhancement of the dielectric constant at low temperatures.

@article{D1TC00785H, abstract = {The electronic properties of molecular conductors can be readily varied via physical or chemical pressure as it enlarges the bandwidth W. This enables them to cross the Mott insulator-to-metal phase transition by reducing electronic correlations U/W. Here we introduce an alternative path by spatially expanding the molecular orbitals when partially replacing sulfur by selenium in the constituting bis-(ethylenedithio)-tetrathiafulvalene (BEDT-TTF) molecules of the title compound. We characterize how the insulating quantum-spin-liquid state is tuned via a Mott transition to the metallic Fermi-liquid state crossing a narrow region of superconductivity. The transport{,} dielectric{,} and optical measurements reveal that at this first-order phase transition{,} metallic regions coexist in the insulating matrix leading to pronounced percolative effects{,} which are most obvious in the strong enhancement of the dielectric constant at low temperatures.}, added-at = {2021-08-31T09:01:59.000+0200}, author = {Saito, Yohei and Rösslhuber, Roland and Löhle, Anja and Sanz Alonso, Miriam and Wenzel, Maxim and Kawamoto, Atsushi and Pustogow, Andrej and Dressel, Martin}, biburl = {https://puma.ub.uni-stuttgart.de/bibtex/282ab23d92f474376924c16d5aeccc1f5/dr.helgakumric}, doi = {10.1039/D1TC00785H}, interhash = {4e93747876e6a98083d6aad608f249cb}, intrahash = {82ab23d92f474376924c16d5aeccc1f5}, journal = {J. Mater. Chem. C}, keywords = {chemical-tuning-molecular-quantum-materials}, number = 33, pages = {10841-10850}, publisher = {The Royal Society of Chemistry}, timestamp = {2021-08-31T07:01:59.000+0200}, title = {Chemical tuning of molecular quantum materials κ-[(BEDT-TTF)1−x(BEDT-STF)x]2Cu2(CN)3: from the Mott-insulating quantum spin liquid to metallic Fermi liquid}, url = {http://dx.doi.org/10.1039/D1TC00785H}, volume = 9, year = 2021 }