Abstract Graphene is a privileged 2D platform for hosting confined light-matter excitations known as surface plasmon polaritons (SPPs), as it possesses low intrinsic losses and a high degree of optical confinement. However, the isotropic nature of graphene limits its ability to guide and focus SPPs, making it less suitable than anisotropic elliptical and hyperbolic materials for polaritonic lensing and canalization. Here, we present graphene/CrSBr as an engineered 2D interface that hosts highly anisotropic SPP propagation across mid-infrared and terahertz energies. Using scanning tunneling microscopy, scattering-type scanning near-field optical microscopy, and first-principles calculations, we demonstrate mutual doping in excess of 1013 cm–2 holes/electrons between the interfacial layers of graphene/CrSBr. SPPs in graphene activated by charge transfer interact with charge-induced electronic anisotropy in the interfacial doped CrSBr, leading to preferential SPP propagation along the quasi-1D chains that compose each CrSBr layer. This multifaceted proximity effect both creates SPPs and endows them with anisotropic propagation lengths that differ by an order-of-magnitude between the in-plane crystallographic axes of CrSBr.

Two-dimensional materials are extraordinarily sensitive to external stimuli, making them ideal for studying fundamental properties and for engineering devices with new functionalities. One such stimulus, strain, affects the magnetic properties of the layered magnetic semiconductor CrSBr to such a degree that it can induce a reversible antiferromagnetic-to-ferromagnetic phase transition. Using scanning SQUID-on-lever microscopy, we directly image the effects of spatially inhomogeneous strain on the magnetization of layered CrSBr, as it is polarized by a field applied along its easy axis. The evolution of this magnetization and the formation of domains is reproduced by a micromagnetic model, which incorporates the spatially varying strain and the corresponding changes in the local interlayer exchange stiffness. The observed sensitivity to small strain gradients along with similar images of a nominally unstrained CrSBr sample suggest that unintentional strain inhomogeneity influences the magnetic behavior of exfoliated samples.

Heavy-fermion metals are prototype systems for observing emergent quantum phases driven by electronic interactions 1 – 6 . A long-standing aspiration is the dimensional reduction of these materials to exert control over their quantum phases 7 – 11 , which remains a significant challenge because traditional intermetallic heavy-fermion compounds have three-dimensional atomic and electronic structures. Here we report comprehensive thermodynamic and spectroscopic evidence of an antiferromagnetically ordered heavy-fermion ground state in CeSiI, an intermetallic comprising two-dimensional (2D) metallic sheets held together by weak interlayer van der Waals (vdW) interactions. Owing to its vdW nature, CeSiI has a quasi-2D electronic structure, and we can control its physical dimension through exfoliation. The emergence of coherent hybridization of f and conduction electrons at low temperature is supported by the temperature evolution of angle-resolved photoemission and scanning tunnelling spectra near the Fermi level and by heat capacity measurements. Electrical transport measurements on few-layer flakes reveal heavy-fermion behaviour and magnetic order down to the ultra-thin regime. Our work establishes CeSiI and related materials as a unique platform for studying dimensionally confined heavy fermions in bulk crystals and employing 2D device fabrication techniques and vdW heterostructures 12 to manipulate the interplay between Kondo screening, magnetic order and proximity effects.

The electronic properties of crystals can be manipulated by superimposing spatially periodic electric, magnetic or structural modulations. Long-wavelength modulations incommensurate with the atomic lattice are particularly interesting1, exemplified by recent advances in two-dimensional (2D) moir & eacute; materials2,3. Bulk van der Waals (vdW) superlattices4-8 hosting 2D interfaces between minimally disordered layers represent scalable bulk analogues of artificial vdW heterostructures and present a complementary venue to explore incommensurately modulated 2D states. Here we report the bulk vdW superlattice SrTa2S5 realizing an incommensurate one-dimensional (1D) structural modulation of 2D transition metal dichalcogenide (TMD) H-TaS2 layers. High-quality electronic transport in the H-TaS2 layers, evidenced by quantum oscillations, is made anisotropic by the modulation and exhibits commensurability oscillations paralleling lithographically modulated 2D systems9-11. We also find unconventional, clean-limit superconductivity in SrTa2S5 with a pronounced suppression of interlayer relative to intralayer coherence. The in-plane magnetic field dependence of interlayer critical current, together with electron diffraction from the structural modulation, suggests superconductivity12-14 in SrTa2S5 is spatially modulated and mismatched between adjacent TMD layers. With phenomenology suggestive of pair-density wave superconductivity15-17, SrTa2S5 may present a pathway for microscopic evaluation of this unconventional order18-21. More broadly, SrTa2S5 establishes bulk vdW superlattices as versatile platforms to address long-standing predictions surrounding modulated electronic phases in the form of nanoscale vdW devices12,13 to macroscopic crystals22,23. Evidence of modulated metallic and superconducting states stemming from an incommensurate structural stripe motif is reported in the bulk van der Waals superlattice SrTa2S5.

Electronic properties of crystals can be manipulated using spatially periodic modulations. Long-wavelength, incommensurate modulations are of particular interest, exemplified recently by moiré patterned van der Waals (vdW) heterostructures. Bulk vdW superlattices hosting interfaces between clean 2D layers represent scalable bulk analogs of vdW heterostructures and present a complementary venue to explore incommensurately modulated 2D states. Here we report the bulk vdW superlattice SrTa$_2$S$_5$ realizing an incommensurate 1D modulation of 2D transition metal dichalcogenide (TMD) $H$-TaS$_2$ layers. High-quality electronic transport in the $H$-TaS$_2$ layers, evidenced by quantum oscillations, is made anisotropic by the modulation and shows commensurability oscillations akin to lithographically modulated 2D systems. We also find unconventional, clean-limit superconductivity (SC) in SrTa$_2$S$_5$ with a pronounced suppression of interlayer coherence relative to intralayer coherence. Such a hierarchy can arise from pair-density wave (PDW) SC with mismatched spatial arrangement in adjacent superconducting layers. Examining the in-plane magnetic field $H_{ab}$ dependence of interlayer critical current density $J_c$, we find anisotropy with respect to $H_{ab}$ orientation: $J_c$ is maximized (minimized) when $H_{ab}$ is perpendicular (parallel) to the stripes, consistent with 1D PDW SC. From diffraction we find the structural modulation is shifted between adjacent $H$-TaS$_2$ layers, suggesting mismatched 1D PDW is seeded by the striped structure. With a high-mobility Fermi liquid in a coherently modulated structure, SrTa$_2$S$_5$ is a promising host for novel phenomena anticipated in clean, striped metals and superconductors. More broadly, SrTa$_2$S$_5$ establishes bulk vdW superlattices as macroscopic platforms to address long-standing predictions for modulated electronic phases.

Graphene is a privileged 2D platform for hosting confined light-matter excitations known as surface plasmon-polaritons (SPPs), as it possesses low intrinsic losses with a high degree of optical confinement. However, the inherently isotropic optical properties of graphene limit its ability to guide and focus SPPs, making it less suitable than anisotropic elliptical and hyperbolic materials as a platform for polaritonic lensing and canalization. Here, we present the graphene/CrSBr heterostructure as an engineered 2D interface that hosts highly anisotropic SPP propagation over a wide range of frequencies in the mid-infrared and terahertz. Using a combination of scanning tunneling microscopy (STM), scattering-type scanning near-field optical microscopy (s-SNOM), and first-principles calculations, we demonstrate mutual doping in excess of 10^13 cm^-2 holes/electrons between the interfacial layers of graphene/CrSBr heterostructures. SPPs in graphene activated by charge transfer interact with charge-induced anisotropic intra- and interband transitions in the interfacial doped CrSBr, leading to preferential SPP propagation along the quasi-1D chains that compose each CrSBr layer. This multifaceted proximity effect both creates SPPs and endows them with anisotropic transport and propagation lengths that differ by an order-of-magnitude between the two in-plane crystallographic axes of CrSBr.

Materials hosting flat electronic bands are a central focus of condensed matter physics as promising venues for novel electronic ground states. Two-dimensional (2D) geometrically frustrated lattices such as the kagome, dice, and Lieb lattices are attractive targets in this direction, anticipated to realize perfectly flat bands. Synthesizing these special structures, however, poses a formidable challenge, exemplified by the absence of solid-state materials realizing the dice and Lieb lattices. An alternative route leverages atomic orbitals to create the characteristic electron hopping of geometrically frustrated lattices. This strategy promises to expand the list of candidate materials to simpler structures, but is yet to be demonstrated experimentally. Here, we report the realization of frustrated hopping in the van der Waals (vdW) intermetallic Pd_5AlI_2, emerging from orbital decoration of a primitive square lattice. Using angle-resolved photoemission spectroscopy and quantum oscillations measurements, we demonstrate that the band structure of Pd_5AlI_2 includes linear Dirac-like bands intersected at their crossing point by a flat band, essential characteristics of frustrated hopping in the Lieb and dice lattices. Moreover, Pd_5AlI_2 is exceptionally stable, with the unusual bulk band structure and metallicity persisting in ambient conditions down to the monolayer limit. Our ability to realize an electronic structure characteristic of geometrically frustrated lattices establishes orbital decoration of primitive lattices as a new approach towards electronic structures that remain elusive to prevailing lattice-centric searches.

Bound states in the continuum (BICs) are quantum states that remain localized despite existing within a continuum of extended, delocalized states. They defy conventional wave theories and could be instrumental for quantum technologies that rely on the precise control of quantum states. While optical BICs have been realized in photonic systems, achieving electronic bound states in a metallic background remains an ongoing challenge. Here, we observe two defect states that remain localized within the metallic continuum of Pd5AlI2, a two-dimensional van der Waals metal. The emergence of these states is a manifestation of the hopping interference in the Pd5AlI2 lattice. This interference results in a (quasi) flat band and spatially localized eigenstates that are orthogonal to the metallic continuum thus avoiding hybridization with extended states.

Atomically thin transition metal dichalcogenides can exhibit markedly different electronic properties compared to their bulk counterparts. In the case of NbSe$_2$, the question of whether its charge density wave (CDW) phase is enhanced in the monolayer limit has been the subject of intense debate, primarily due to the difficulty of decoupling this order from its environment. Here, we address this challenge by using a misfit crystal that comprises NbSe$_2$ monolayers separated by SnSe rock-salt spacers, a structure that allows us to investigate a monolayer crystal embedded in a bulk matrix. We establish an effective monolayer electronic behavior of the misfit crystal by studying its transport properties and visualizing its electronic structure by angle-resolved photoemission measurements. We then investigate the emergence of the CDW by tracking the temperature dependence of its collective modes. Our findings reveal a nearly sixfold enhancement in the CDW transition temperature, providing compelling evidence for the profound impact of dimensionality on charge order formation in NbSe$_2$.

Journal Article Methods for Multi-Layer van der Waals Heterostructures Topological Materials Discovery via STEM and LEEM Get access David C Bell, David C Bell Harvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA USA Search for other works by this author on: Oxford Academic Google Scholar Cigdem Ozsoy-Keskinbora, Cigdem Ozsoy-Keskinbora Harvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA USA Search for other works by this author on: Oxford Academic Google Scholar Austin Akey, Austin Akey Center for Nanoscale Systems, Harvard University, Cambridge, MA, USA Search for other works by this author on: Oxford Academic Google Scholar Aravind Devarakonda, Aravind Devarakonda Department of Physics, MIT Cambridge, MA, USADepartment of Physics, MIT Cambridge, MA, USA Search for other works by this author on: Oxford Academic Google Scholar Liang Fu, Liang Fu Department of Physics, MIT Cambridge, MA, USA Search for other works by this author on: Oxford Academic Google Scholar Efthimios Kaxiras, Efthimios Kaxiras Department of Physics, Harvard University, Cambridge, MA, USA Search for other works by this author on: Oxford Academic Google Scholar Joseph Checkelsky Joseph Checkelsky Department of Physics, MIT Cambridge, MA, USA Search for other works by this author on: Oxford Academic Google Scholar Microscopy and Microanalysis, Volume 28, Issue S1, 1 August 2022, Pages 1702–1703, https://doi.org/10.1017/S1431927622006754 Published: 01 August 2022

The discovery of extraordinary new quantum materials with striking properties has caused great excitement and promises to transform signal processing and computation. We have performed integrated research on three materials. Remarkably, the quantum phenomena displayed by these materials persists at room temperature, changing the rules for signal processing and computation and opening the way for quantum electronics.

Charged particles subjected to magnetic fields form Landau levels (LLs). Originally studied in the context of electrons in metals 1 , fermionic LLs continue to attract interest as hosts of exotic electronic phenomena 2 , 3 . Bosonic LLs are also expected to realize novel quantum phenomena 4 , 5 , but, apart from recent advances in synthetic systems 6 , 7 , they remain relatively unexplored. Cooper pairs in superconductors—composite bosons formed by electrons—represent a potential condensed-matter platform for bosonic LLs. Under certain conditions, an applied magnetic field is expected to stabilize an unusual superconductor with finite-momentum Cooper pairs 8 , 9 and exert control over bosonic LLs 10 – 13 . Here we report thermodynamic signatures, observed by torque magnetometry, of bosonic LL transitions in the layered superconductor Ba 6 Nb 11 S 28 . By applying an in-plane magnetic field, we observe an abrupt, partial suppression of diamagnetism below the upper critical magnetic field, which is suggestive of an emergent phase within the superconducting state. With increasing out-of-plane magnetic field, we observe a series of sharp modulations in the upper critical magnetic field that are indicative of distinct vortex states and with a structure that agrees with predictions for Cooper pair LL transitions in a finite-momentum superconductor 10 – 14 . By applying Onsager’s quantization rule 15 , we extract the momentum. Furthermore, study of the fermionic LLs shows evidence for a non-zero Berry phase. This suggests opportunities to study bosonic LLs, topological superconductivity, and their interplay via transport 16 , scattering 17 , scanning probe 18 and exfoliation techniques 19 .

Quantum Materials may act as conductors, insulators, semiconductors or even as superconductors. Especially, combinations of different quantum materials are of high interest to explore new phenomena and to build the foundation for future electronic devices at the nanometer scale. The properties of quantum materials differ strongly from the properties of their three-dimensional bulk state. Our research on quantum materials is widely spread, reaching from defect formation in graphene to the characterization of hybrid quantum materials. We use low voltage aberration corrected electron microscopy to investigate chemical various quantum materials. In particular, we will present imaging and analysis of vapor deposition (CVD) graphene with added copper and mercury defects; graphene based hybrid structures, and FeSn Topological Insulators.

Advances in low-dimensional superconductivity are often realized through improvements in material quality. Apart from a small group of organic materials, there is a near absence of clean-limit two-dimensional (2D) superconductors, which presents an impediment to the pursuit of numerous long-standing predictions for exotic superconductivity with fragile pairing symmetries. We developed a bulk superlattice consisting of the transition metal dichalcogenide (TMD) superconductor 2H-niobium disulfide (2H-NbS2) and a commensurate block layer that yields enhanced two-dimensionality, high electronic quality, and clean-limit inorganic 2D superconductivity. The structure of this material may naturally be extended to generate a distinct family of 2D superconductors, topological insulators, and excitonic systems based on TMDs with improved material properties.

The recent development of two-dimensional (2D) van der Waals (vdW) materials has enabled the rapid exploration of novel low-dimensional electronic phenomena. The family of hexagonal transition metal dichalcogenides ($H$-$MX_2$) has proven to be a particularly rich host of exotic quantum phases due to their crystal structure and strong spin-orbit coupling. However, these materials are often subject to degradation, and for exfoliated materials, reduction in quality during the fabrication process can constrain the phase space for potential ground states. Here we show that high-quality $H$-NbS$_2$ monolayers with electronic mobilities more than three orders of magnitude larger than in bulk $2H$-NbS$_{2}$ can be realized in a bulk single crystal superlattice formed with a commensurate block layer. We find that these materials are clean-limt 2D superconductors exhibiting a Berezinskii-Kosterlitz-Thouless (BKT) transition at $T_{BKT} = 0.82$ K and prominent 2D Shubnikov de-Haas quantum oscillations. Furthermore, we observe an enhancement of the superconducting upper critical field $\mu_0H_{c2}$ beyond the Pauli limit for field applied within a narrow angular window $\delta \theta \lesssim 2^\circ$ of the layer plane, which we show is consistent with field-induced finite momentum Cooper pairing enhanced by local symmetry breaking. Our results demonstrate the ability of these commensurate superlattices to support clean monolayer $H$-$MX_2$ beyond that possible in their bulk $2H$-$MX_2$ counterparts and monolayers exfoliated therefrom. Their structure and exfoliability offer pathways to direct probing of pair density wave superconductivity and, more broadly, the possibility of engineering other high quality 2D $MX_2$ layers in a new class of bulk single crystal superlattices.

Virtual Reality (VR) offers advantages for learning and research when dealing with concepts or systems that are highly spatial. The ability to gain a new perspective by moving the head or by using the hands to manipulate an object is highly intuitive and allows learners to focus on the subject matter rather than the interface. Even so, many obstacles remain for this potential to be reaped at scale and across disciplines in formal educational and research settings. Here we describe an end-to-end effort to create and implement an immersive tool for learning and research that would overcome these obstacles and prove practically usable and useful in such contexts. The creation process required overcoming myriad design and engineering challenges — these and our corresponding approaches are described in detail.

Quantum Materials may act as conductors, insulators, semiconductors or even as superconductors.Especially combinations of different quantum materials are of high interest to explore new phenomena and to build the foundation for future electronic devices at the nanometer scale.The properties of quantum materials differ strongly from the properties of their three dimensional bulk state.Our research on quantum materials is widely spread, reaching from defect formation in graphene to the characterization of hybrid quantum materials.We use low voltage aberration corrected electron microscopy to investigate chemical various quantum materials.In particular, we will present imaging and analysis of vapor deposition (CVD) graphene with added copper and mercury defects; graphene based hybrid structures, and FeSn Topological Insulators.

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