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We find evidence for the formation and relaxation of large exciton polarons in 2D organic-inorganic hybrid perovskites. Using ps-scale time-resolved photoluminescence within the phenethylammonium lead iodide family of compounds, we identify a red shifting of emission that we associate with exciton polaron formation time scales of 3-10 ps. Atomic substitutions of the phenethylammonium cation allow local control over the structure of the inorganic lattice, and we show that the structural differences among materials strongly influence the exciton polaron relaxation process, revealing a polaron binding energy that grows larger (up to 15 meV) in more strongly distorted compounds.

We investigated Xe binding in a previously reported paramagnetic metal–organic tetrahedral capsule, [Co4L6]4–, where L2– = 4,4′-bis[(2-pyridinylmethylene)amino][1,1′-biphenyl]-2,2′-disulfonate. The...

We report a family of two-dimensional hybrid perovskites (2DHPs) based on phenethylammonium lead iodide ((PEA)$_2$PbI$_4$) that show complex structure in their low-temperature excitonic absorption and photoluminescence (PL) spectra as well as hot exciton PL. We replace the 2-position (ortho) H on the phenyl group of the PEA cation with F, Cl, or Br to systematically increase the cation's cross-sectional area and mass and study changes in the excitonic structure. These single atom substitutions substantially change the observable number of and spacing between discrete resonances in the excitonic absorption and PL spectra and drastically increase the amount of hot exciton PL that violates Kasha's rule by over an order of magnitude. To fit the progressively larger cations, the inorganic framework distorts and is strained, reducing the Pb-I-Pb bond angles and increasing the 2DHP band gap. Correlation between the 2DHP structure and steady-state and time-resolved spectra suggests the complex structure of resonances arises from one or two manifolds of states, depending on the 2DHP Pb-I-Pb bond angle (as)symmetry, and the resonances within a manifold are regularly spaced with an energy separation that decreases as the mass of the cation increases. The uniform separation between resonances and the dynamics that show excitons can only relax to the next-lowest state are consistent with a vibronic progression caused by a vibrational mode on the cation. These results demonstrate that simple changes to the structure of the cation can be used to tailor the properties and dynamics of the confined excitons without directly modifying the inorganic framework., Comment: 39 pages

The properties of van der Waals (vdW) materials often vary dramatically with the atomic stacking order between layers, but this order can be difficult to control. Trilayer graphene (TLG) stacks in either a semimetallic ABA or a semiconducting ABC configuration with a gate-tunable band gap, but the latter has only been produced by exfoliation. Here we present a chemical vapor deposition approach to TLG growth that yields greatly enhanced fraction and size of ABC domains. The key insight is that substrate curvature can stabilize ABC domains. Controllable ABC yields ~59% were achieved by tailoring substrate curvature levels. ABC fractions remained high after transfer to device substrates, as confirmed by transport measurements revealing the expected tunable ABC band gap. Substrate topography engineering provides a path to large-scale synthesis of epitaxial ABC-TLG and other vdW materials., We thank Prof. Paul Heiney for useful discussions and Mr. Sheng Wang for help in creating Fig. 4a. This work was supported by the NSF EFRI 2-DARE 1542879. The Synchrotron SOLEIL is supported by the Centre National de la Recherche Scientifique (CNRS) and the Commissariat `a l’Energie Atomique et aux Energies Alternatives (CEA), France. J.B. and D.J.S. thank Jian Han for useful discussions and were supported as part of the Center for the Computational Design of Functional Layered Materials, an Energy Frontier Research Center funded by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES) under Award DE-SC0012575. Part of J.B.ʼs contribution was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. W.P. and M.D. acknowledge support from the NSF EFRI 2-DARE 1542707 and NSF EAGER 1838456. Z.L. appreciates support by the NSFC-RGC Joint Research Scheme (N_HKUST607/17) and the Guangzhou Science and Technology Project (201704030134). J.G. thanks the German Research Council (DFG) for support via grants GE2827/1-1 and GE2827/2-1. J.M.K. thanks the support from NSF MRSEC DMR-1720530. The infrared near-field nanoscopy measurements is supported by the Director, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division of the U.S. Department of Energy under Contract No. DE-AC02-05-CH11231 (Sub-wavelength Metamaterial program). A.M.R. acknowledges support of the National Science Foundation, under Grant DMR-1719353.

Evolution of Kondo effect in Weyl semimetal Mn3Sn leads to extraordinary terahertz and DC transport properties., Topology and strong electron correlations are crucial ingredients in emerging quantum materials, yet their intersection in experimental systems has been relatively limited to date. Strongly correlated Weyl semimetals, particularly when magnetism is incorporated, offer a unique and fertile platform to explore emergent phenomena in novel topological matter and topological spintronics. The antiferromagnetic Weyl semimetal Mn3Sn exhibits many exotic physical properties such as a large spontaneous Hall effect and has recently attracted intense interest. In this work, we report synthesis of epitaxial Mn3+xSn1−x films with greatly extended compositional range in comparison with that of bulk samples. As Sn atoms are replaced by magnetic Mn atoms, the Kondo effect, which is a celebrated example of strong correlations, emerges, develops coherence, and induces a hybridization energy gap. The magnetic doping and gap opening lead to rich extraordinary properties, as exemplified by the prominent DC Hall effects and resonance-enhanced terahertz Faraday rotation.

The topological kagome magnet (TKM) Fe3Sn2 exhibits unusual topological properties, flat electronic bands, and chiral spin textures, making it an exquisite materials platform to explore the interplay between topological band structure, strong electron correlations, and magnetism. Here we report the first synthesis of high-quality epitaxial (0001) Fe3Sn2 films with large intrinsic anomalous Hall effect close to that measured in bulk single crystals. In addition, we measured a large, anisotropic anomalous Nernst coefficient Syx of 1.26 {\mu}V/K, roughly 2-5x greater than that of common ferromagnets, suggesting the presence of Berry curvature sources near the Fermi level in this system. Crucially, the realization of high-quality Fe3Sn2 films opens the door to explore emergent interfacial physics and create novel spintronic devices based on TKMs by interfacing Fe3Sn2 with other quantum materials and by nanostructure patterning., Comment: accepted by Physical Review Materials

Topology and strong electron correlations are crucial ingredients in emerging quantum materials, yet their intersection in experimental systems has been relatively limited to date. Strongly correlated Weyl semimetals, particularly when magnetism is incorporated, offer a unique and fertile platform to explore emergent phenomena in novel topological matter and topological spintronics. The antiferromagnetic Weyl semimetal Mn3Sn exhibits many exotic physical properties such as a large spontaneous Hall effect and has recently attracted intense interest. In this work, we report synthesis of epitaxial Mn3+x Sn1-x films with greatly extended compositional range in comparison with that of bulk samples. As Sn atoms are replaced by magnetic Mn atoms, the Kondo effect, which is a celebrated example of strong correlations, emerges, develops coherence, and induces a hybridization energy gap. The magnetic doping and gap opening lead to rich extraordinary properties, as exemplified by the prominent DC Hall effects and resonance-enhanced terahertz Faraday rotation.

The topological kagome metal CoSn hosts orbital-selective Dirac bands and very flat bands near the Fermi energy that lead to a range of exotic phenomena, such as fractional quantum Hall states. In this work, we report the synthesis of high-quality epitaxial (0001) CoSn films by magnetron sputtering. Comprehensive structural characterizations demonstrate high crystalline quality with low disorder, sharp interfaces, and a smooth surface. Complementary magnetic and transport properties show a paramagnetic, metallic ground state as seen in bulk. Our work creates a synthetic foundation to investigate and utilize rich topological physics in CoSn thin films and heterostructures.

Quantum and dielectric confinement effects in Ruddlesden-Popper 2D hybrid perovskites create excitons with a binding energy exceeding 150 meV. We exploit the large exciton binding energy to study exciton and carrier dynamics as well as electron-phonon coupling (EPC) in hybrid perovskites using absorption and photoluminescence (PL) spectroscopies. At temperatures75 K, we resolve splitting of the excitonic absorption and PL into multiple regularly spaced resonances every 40-46 meV, consistent with EPC to phonons located on the organic cation. We also resolve resonances with a 14 meV spacing, in accord with coupling to phonons with mixed organic and inorganic character. These assignments are supported by density-functional theory calculations. Hot exciton PL and time-resolved PL measurements show that vibrational relaxation occurs on a picosecond time scale competitive with that for PL. At temperatures75 K, excitonic absorption and PL exhibit homogeneous broadening. While absorption remains homogeneous, PL becomes inhomogeneous at temperatures75K, which we speculate is caused by the formation and subsequent dynamics of a polaronic exciton.