Search for: All records

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 10¹³cm^–2holes/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. 

It is undeniable that novel 2D devices and heterostructures will have a lasting impact on the advancement of future technologies. However, the inherent instability of many exfoliated van der Waals (vdW) materials is a well-known hurdle yet to be overcome. Thus, the sustained interest in exfoliated vdW materials underscores the importance of understanding the mechanisms of sample degradation to establish proactive protective measures. Here, the impact of prolonged synchrotron-based X-ray beam exposure on exfoliated flakes of two contemporary vdW materials, ${\mathrm{N}\mathrm{i}\mathrm{P}\mathrm{S}}_3$and $\alpha$- ${\mathrm{R}\mathrm{u}\mathrm{C}\mathrm{l}}_3$, is explored using resonant inelastic X-ray scattering (RIXS) and total fluorescence yield X-ray absorption spectroscopy (XAS). In ${\mathrm{N}\mathrm{i}\mathrm{P}\mathrm{S}}_3$, the resulting RIXS and XAS spectra show a suppression, then vanishing, of NiS₆multiplet excitations coupled with an upward shift of the peak energy of the XAS as a function of X-ray dose. In $\alpha$- ${\mathrm{R}\mathrm{u}\mathrm{C}\mathrm{l}}_3$, the signs of beam damage from the RIXS spectra are less evident. However, the post-experiment characterization of both materials using Raman spectroscopy exhibits signals of an amorphous and disordered system compared to pristine flakes; in addition, energy-dispersive X-ray spectroscopy of ${\mathrm{N}\mathrm{i}\mathrm{P}\mathrm{S}}_3$shows evidence of ligand vacancies. As synchrotron radiation is fast becoming a required probe to study 2D vdW materials, these findings lay the groundwork for the development of future protective measures for synchrotron-based prolonged X-ray beam exposure, as well as for X-ray free electron laser. 

We present a basic framework for modeling collective mode effects in photocurrent measurements performed on two-dimensional materials using nano-optical scanned probes. We consider photothermal, photovoltaic, and bolometric contributions to the photocurrent. We show that any one of these can dominate depending on frequency, temperature, applied bias, and sample geometry. Our model is able to account for periodic spatial oscillations (fringes) of the photocurrent observed near sample edges or inhomogeneities. For the case of a non-absorbing substrate, we find a direct relation between the spectra measured by the photocurrent nanoscopy and its parental scanning technique near-field optical microscopy. 

Topological semimetals with massless Dirac and Weyl fermions represent the forefront of quantum materials research. In two dimensions, a peculiar class of fermions that are massless in one direction and massive in the perpendicular direction was predicted 16 years ago. These highly exotic quasiparticles—the semi-Dirac fermions—ignited intense theoretical and experimental interest but remain undetected. Using magneto-optical spectroscopy, we demonstrate the defining feature of semi-Dirac fermions— $B^{2/3}$scaling of Landau levels—in a prototypical nodal-line metal ZrSiS. In topological metals, including ZrSiS, nodal lines extend the band degeneracies from isolated points to lines, loops, or even chains in the momentum space. With calculations and theoretical modeling, we pinpoint the observed semi-Dirac spectrum to the crossing points of nodal lines in ZrSiS. Crossing nodal lines exhibit a continuum absorption spectrum but with singularities that scale as $B^{2/3}$at the crossing. Our work sheds light on the hidden quasiparticles emerging from the intricate topology of crossing nodal lines and highlights the potential to explore quantum geometry with linear optical responses. Published by the American Physical Society2024 

Ultraclean graphene at charge neutrality hosts a quantum critical Dirac fluid of interacting electrons and holes. Interactions profoundly affect the charge dynamics of graphene, which is encoded in the properties of its electron-photon collective modes: surface plasmon polaritons (SPPs). Here, we show that polaritonic interference patterns are particularly well suited to unveil the interactions in Dirac fluids by tracking polaritonic interference in time at temporal scales commensurate with the electronic scattering. Spacetime SPP interference patterns recorded in terahertz (THz) frequency range provided unobstructed readouts of the group velocity and lifetime of polariton that can be directly mapped onto the electronic spectral weight and the relaxation rate. Our data uncovered prominent departures of the electron dynamics from the predictions of the conventional Fermi-liquid theory. The deviations are particularly strong when the densities of electrons and holes are approximately equal. The proposed spacetime imaging methodology can be broadly applied to probe the electrodynamics of quantum materials.