skip to main content


Title: Revealing Phonon Polaritons in Hexagonal Boron Nitride by Multipulse Peak Force Infrared Microscopy
Abstract

Probing of polaritons in 2D materials is facilitated by spectroscopic imaging with nanometer spatial resolution. The combination of atomic force microscopy and infrared laser sources provides access for in situ mappings of phonon polaritons. Here, it is demonstrated that the photothermal‐based peak force infrared microscopy is capable of revealing phonon polaritons with high spatial resolution in isotopically pure hexagonal boron nitride microstructures without damaging the sample. To further improve the sensitivity, peak force infrared microscopy is enhanced with a scheme of multiple laser pulse excitation. The resulting method of multipulse peak force infrared microscopy can detect phonon polaritons with high sensitivity, which is particularly useful for probing polaritons in 2D materials with high damping characteristics.

 
more » « less
Award ID(s):
1852010 1359195 1847765
NSF-PAR ID:
10457672
Author(s) / Creator(s):
 ;  ;  ;  ;  ;  ;  
Publisher / Repository:
Wiley Blackwell (John Wiley & Sons)
Date Published:
Journal Name:
Advanced Optical Materials
Volume:
8
Issue:
5
ISSN:
2195-1071
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    We selectively excite and study two new types of phonon-polariton guided modes that are found in hexagonal boron nitride thin flakes on a gold substrate. Such modes show substantially improved confinement and a group velocity that is hundreds of times slower than the speed of light, thereby providing a new way to create slow light in the mid-infrared range with a simple structure that does not require nano-patterning. One mode is the fundamental mode in the first Restrahlen band of hexagonal boron nitride thin crystals on a gold substrate; the other mode is equivalent to the second mode of the second Restrahlen band of hexagonal boron nitride flakes that are suspended in vacuum.

    The new modes also couple efficiently with incident light at the hexagonal boron nitride edges, as we demonstrate experimentally using photo-induced force microscopy and scanning near-field optical microscopy. The high confinement of these modes allows for Purcell factors that are on the order of tens of thousands directly above boron nitride and a wide band, with new perspectives for enhanced light-matter interaction. Our findings demonstrate a new approach to engineering the dispersion of polaritons in 2D materials to improve confinement and light-matter interaction, thereby paving the way for new applications in mid-infrared nano-optics.

     
    more » « less
  2. Abstract

    2D van der Waals (vdW) materials are emerging as the next generation platform for optical and electronic devices with their wide coverage of the energy bandgaps. The strong light–matter interactions in 2D vdW layers allow for exploring novel optical and electronic phenomena such as 2D polaritons exhibiting ultrahigh field confinement, defects‐induced new quantum states, and strain‐modulated quantum confinement of 2D excitons. Far‐field optical imaging techniques are extensively used to characterize the 2D vdW materials so far, however, subdiffraction spatial resolution is required for comprehensive investigations of 2D vdW materials of which physical properties are greatly influenced by local defects and strain. This article aims to cover historical advances, fundamental principles, and distinct features of emerging near‐field optical imaging techniques: scattering‐type scanning near‐field optical microscopy, tip‐enhanced Raman spectroscopy, tip‐enhanced photoluminescence techniques, and photo‐induced force microscopy. The recent developments toward spectroscopic analysis of near‐field imaging and applications for unveiling unique properties of 2D polaritons, nanoscale defects, and mechanical strains in 2D vdW materials, are also discussed. This review article provides an understanding of emerging near‐field imaging techniques and suggests prospective applications for exploring 2D vdW materials.

     
    more » « less
  3. Coherent optical excitations in two-dimensional (2D) materials, 2D polaritons, can generate a plethora of optical phenomena that arise from the extraordinary dispersion relations that do not exist in regular materials. Probing of the dynamical phenomena of 2D polaritons requires simultaneous spatial and temporal imaging capabilities and could reveal unknown coherent optical phenomena in 2D materials. Here, we present a spatiotemporal measurement of 2D wave packet dynamics, from its formation to its decay, using an ultrafast transmission electron microscope driven by femtosecond midinfrared pulses. The ability to coherently excite phonon-polariton wave packets and probe their evolution in a nondestructive manner reveals intriguing dispersion-dependent dynamics that includes splitting of multibranch wave packets and, unexpectedly, wave packet deceleration and acceleration. Having access to the full spatiotemporal dynamics of 2D wave packets can be used to illuminate puzzles in topological polaritons and discover exotic nonlinear optical phenomena in 2D materials.

     
    more » « less
  4. Abstract

    Structural anisotropy in crystals is crucial for controlling light propagation, particularly in the infrared spectral regime where optical frequencies overlap with crystalline lattice resonances, enabling light-matter coupled quasiparticles called phonon polaritons (PhPs). Exploring PhPs in anisotropic materials like hBN and MoO3has led to advancements in light confinement and manipulation. In a recent study, PhPs in the monoclinic crystal β-Ga2O3(bGO) were shown to exhibit strongly asymmetric propagation with a frequency dispersive optical axis. Here, using scanning near-field optical microscopy (s-SNOM), we directly image the symmetry-broken propagation of hyperbolic shear polaritons in bGO. Further, we demonstrate the control and enhancement of shear-induced propagation asymmetry by varying the incident laser orientation and polariton momentum using different sizes of nano-antennas. Finally, we observe significant rotation of the hyperbola axis by changing the frequency of incident light. Our findings lay the groundwork for the widespread utilization and implementation of polaritons in low-symmetry crystals.

     
    more » « less
  5. Abstract

    Correlative scanning probe microscopy of chemical identity, surface potential, and mechanical properties provide insight into the structure–function relationships of nanomaterials. However, simultaneous measurement with comparable and high resolution is a challenge. We seamlessly integrated nanoscale photothermal infrared imaging with Coulomb force detection to form peak force infrared–Kelvin probe force microscopy (PFIR‐KPFM), which enables simultaneous nanomapping of infrared absorption, surface potential, and mechanical properties with approximately 10 nm spatial resolution in a single‐pass scan. MAPbBr3perovskite crystals of different degradation pathways were studied in situ. Nanoscale charge accumulations were observed in MAPbBr3near the boundary to PbBr2. PFIR‐KPFM also revealed correlations between residual charges and secondary conformation in amyloid fibrils. PFIR‐KPFM is applicable to other heterogeneous materials at the nanoscale for correlative multimodal characterizations.

     
    more » « less