Moiré heterostructures of transition metal dichalcogenides (TMDs) exhibit Mott-insulating behavior both at half filling as well as at fractional fillings, where electronic degrees of freedom form self-organized Wigner crystal states. An open question concerns magnetic states obtained by lifting the pseudospin-1/2 degeneracy of these states at lowest temperatures. While at half filling virtual hopping is expected to induce (weak) antiferromagnetic exchange interactions, these are strongly suppressed when considering dilute filling fractions. We argue that, instead, a small concentration of doped electrons leads to the formation of spin polarons, inducing ferromagnetic order at experimentally relevant temperatures, consistent with recently observed ferromagnetic states in moiré TMD systems. We predict explicit signatures of polaron formation in the magnetization profile.
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http://dx.doi.org/10.1103/PhysRevLett.132.046501 | DOI Listing |
Phys Chem Chem Phys
January 2025
Department of Chemical Engineering, Birla Institute of Technology and Science, Pilani, Rajasthan 333031, India.
Naphthalenediimide (NDI)-based donor-acceptor co-polymers with tunable electronic, optical, mechanical, and transport properties have shown immense potential as n-type conducting polymers in organic (opto)electronics. During the operation, the polymers undergo reduction at different charged states, which alters their (opto)electronic properties mainly due to the formation of the quasiparticles, polaron/bipolaron. The theoretical study based on quantum mechanical calculations can provide us with a detailed understanding of their (opto)electronic properties, which is missing to a great extent.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
Chemistry Research Laboratory, Department of Chemistry, University of Oxford, Oxford OX1 3TA, U.K.
The delocalization length of charge carriers in organic semiconductors influences their mobility and is an important factor in the design of functional materials. Here, we have studied the radical anions of a series of linear and cyclic butadiyne-linked porphyrin oligomers using CW-EPR, H Mims ENDOR and NIR/MIR spectroelectrochemistry together with DFT calculations and multiscale molecular modeling. Low-temperature hyperfine EPR spectroscopy and optical data show that polarons are delocalized nonuniformly over about four porphyrins with most of the spin density on just two units even in the cyclic structures, in which all porphyrin sites are identical.
View Article and Find Full Text PDFNat Commun
January 2025
Department of Physics and Arnold Sommerfeld Center for Theoretical Physics (ASC), Ludwig-Maximilians-Universität München, München, Germany.
Proc Natl Acad Sci U S A
December 2024
Stanford Institute for Materials and Energy Sciences, Stanford Linear Accelerator Center (SLAC) National Accelerator Laboratory, Menlo Park, CA 94025.
Recent experiments suggest a new paradigm toward novel colossal magnetoresistance (CMR) in a family of materials EuM[Formula: see text]X[Formula: see text] (M [Formula: see text] Cd, In, Zn; X [Formula: see text] P, As), distinct from the traditional avenues involving Kondo-Ruderman-Kittel-Kasuya-Yosida crossovers, magnetic phase transitions with structural distortions, or topological phase transitions. Here, we use angle-resolved photoemission spectroscopy and density functional theory calculations to explore their origin, particularly focusing on EuCd[Formula: see text]P[Formula: see text]. While the low-energy spectral weight royally tracks that of the resistivity anomaly near the temperature with maximum magnetoresistance ([Formula: see text]) as expected from transport-spectroscopy correspondence, the spectra are completely incoherent and strongly suppressed with no hint of a Landau quasiparticle.
View Article and Find Full Text PDFACS Nano
December 2024
Diamond Light Source, Harwell Science and Innovation Campus, Didcot OX11 0DE, U.K.
Interaction between electrons and phonons in solids is a key effect defining the physical properties of materials, such as electrical and thermal conductivity. In transition metal dichalcogenides (TMDCs), the electron-phonon coupling results in the formation of polarons, quasiparticles that manifest themselves as discrete features in the electronic spectral function. In this study, we report the formation of polarons at the alkali-dosed MoSe surface, where Rashba-like spin splitting of the conduction band states is caused by an inversion-symmetry breaking electric field.
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