Abstract:Twisted two-dimensional van der Waals (vdW) heterostructures have unlocked a new means for manipulating the properties of quantum materials. The resulting mesoscopic moiré superlattices are accessible to a wide variety of scanning probes. To date, spatially-resolved techniques have prioritized electronic structure visualization, with lattice response experiments only in their infancy. Here, we therefore investigate lattice dynamics in twisted layers of hexagonal boron nitride (hBN), formed by a minute twist an… Show more
“…A wide range of emerging electronic, magnetic, and topological properties in quantum materials are intimately linked to spatial inversion symmetry. In van der Waals heterostructures, the crystal symmetry can be precisely controlled by interlayer stacking and twisting techniques, providing a knob for programming the electronic bandstructure, [1][2][3] magnetic orders, [4] optical, [5][6][7][8][9][10][11] thermal [12] and phonon properties, [13] atomic reconstruction, [14] etc. Second harmonic generation (SHG) is the lowest-order nonlinear optical response, where the incident laser beam interacts with the material, emitting a frequency-doubled signal.…”
Second harmonic generation (SHG) is a nonlinear optical response arising exclusively from broken inversion symmetry in the electric‐dipole limit. Recently, SHG has attracted widespread interest as a versatile and noninvasive tool for characterization of crystal symmetry and emerging ferroic or topological orders in quantum materials. However, conventional far‐field optics is unable to probe local symmetry at the deep subwavelength scale. Here, near‐field SHG imaging of 2D semiconductors and heterostructures with the spatial resolution down to 20 nm is demonstrated using a scattering‐type nano‐optical apparatus. It is shown that near‐field SHG efficiency is greatly enhanced by excitons in atomically thin transition metal dichalcogenides. Furthermore, by correlating nonlinear and linear scattering‐type nano‐imaging, nanoscale variations of interlayer stacking order in bilayer WSe2 are resolved, and the stacking‐tuned excitonic light–matter interactions are revealed. This work demonstrates nonlinear optical interrogation of crystal symmetry and structure–property relationships at the nanometer length scales relevant to emerging properties in quantum materials.
“…A wide range of emerging electronic, magnetic, and topological properties in quantum materials are intimately linked to spatial inversion symmetry. In van der Waals heterostructures, the crystal symmetry can be precisely controlled by interlayer stacking and twisting techniques, providing a knob for programming the electronic bandstructure, [1][2][3] magnetic orders, [4] optical, [5][6][7][8][9][10][11] thermal [12] and phonon properties, [13] atomic reconstruction, [14] etc. Second harmonic generation (SHG) is the lowest-order nonlinear optical response, where the incident laser beam interacts with the material, emitting a frequency-doubled signal.…”
Second harmonic generation (SHG) is a nonlinear optical response arising exclusively from broken inversion symmetry in the electric‐dipole limit. Recently, SHG has attracted widespread interest as a versatile and noninvasive tool for characterization of crystal symmetry and emerging ferroic or topological orders in quantum materials. However, conventional far‐field optics is unable to probe local symmetry at the deep subwavelength scale. Here, near‐field SHG imaging of 2D semiconductors and heterostructures with the spatial resolution down to 20 nm is demonstrated using a scattering‐type nano‐optical apparatus. It is shown that near‐field SHG efficiency is greatly enhanced by excitons in atomically thin transition metal dichalcogenides. Furthermore, by correlating nonlinear and linear scattering‐type nano‐imaging, nanoscale variations of interlayer stacking order in bilayer WSe2 are resolved, and the stacking‐tuned excitonic light–matter interactions are revealed. This work demonstrates nonlinear optical interrogation of crystal symmetry and structure–property relationships at the nanometer length scales relevant to emerging properties in quantum materials.
“…For example, scattering near-field optical microscopy (s-SNOM) uncovered the variation of the in-plane optical phonon frequencies for different stacking in the moiré superlattice of a twisted hBN (t-hBN). 24 Piezo force microscopy revealed strain gradients along moiré stacking domain boundaries, through piezoelectric coupling to an electric field applied between atomic force microscope (AFM) tip and hBN sample. 19 Electrostatic force microscopy (EFM) and kelvin probe force microscopy (KPFM) were performed on t-hBN (1–20L-BN on top of a thicker >30L flake 20 ), addressing the existence of two opposite permanent out-of-plane polarizations emerging from the moiré pattern.…”
When a twist angle
is applied between two layered materials (LMs),
the registry of the layers and the associated change in their functional
properties are spatially modulated, and a moiré superlattice
arises. Several works explored the optical, electric, and electromechanical
moiré-dependent properties of such twisted LMs but, to the
best of our knowledge, no direct visualization and quantification
of van der Waals (vdW) interlayer interactions has been presented,
so far. Here, we use tapping mode atomic force microscopy phase-imaging
to probe the spatial modulation of the vdW potential in twisted hexagonal
boron nitride. We find a moiré superlattice in the phase channel
only when noncontact (long-range) forces are probed, revealing the
modulation of the vdW potential at the sample surface, following AB
and BA stacking domains. The creation of scalable electrostatic domains,
modulating the vdW potential at the interface with the environment
by means of layer twisting, could be used for local adhesion engineering
and surface functionalization by affecting the deposition of molecules
or nanoparticles.
“…Extension of these nonlinear effects to polaritonic modes [94][95][96] beyond those in graphene is a meaningful future direction. For example, monolayer hexagonal boron nitride [97,98] should exhibit strong second order optical nonlinearity due to broken inversion symmetry of the crystal lattice, and would be a natural platform for generating entanglement between the long lived hyperbolic phonon polaritons [99][100][101][102][103][104][105][106][107][108]. Similar nonlinear processes exist for optical phonons in SiC [109], Josephson plasmons in layered superconductors [110][111][112][113] and the collective modes in excitonic insulators [114][115][116][117][118].…”
Section: Discussion and Experimental Outlookmentioning
We analyze nonlinear optics schemes for generating pairs of quantum entangled plasmons in graphene. We predict that high plasmonic field concentration and strong optical nonlinearity of monolayer graphene enables pair-generation rates much higher than those of conventional photonic sources. The first scheme we study is spontaneous parametric down conversion in a graphene nanoribbon. In this second-order nonlinear process a plasmon excited by an external pump splits into a pair of plasmons, of half the original frequency each, emitted in opposite directions. The conversion is activated by applying a dc electric field that induces a density gradient or a current across the ribbon. Another scheme is degenerate four-wave mixing where the counter-propagating plasmons are emitted at the pump frequency. This third-order nonlinear process does not require a symmetrybreaking dc field. We suggest nano-optical experiments for measuring position-momentum entanglement of the emitted plasmon pairs. We estimate the critical pump fields at which the plasmon generation rates exceed their dissipation, leading to parametric instabilities.
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