Search arXivSearch

arXiv · 2105.06703

Substrate matters: Surface-polariton enhanced infrared nanospectroscopy of molecular vibrations

Abstract

Infrared nanospectroscopy based on Fourier transform infrared near-field spectroscopy (nano-FTIR) is an emerging nanoanalytical tool with large application potential for label-free mapping and identification of organic and inorganic materials with nanoscale spatial resolution. However, the detection of thin molecular layers and nanostructures on standard substrates is still challenged by weak signals. Here, we demonstrate a significant enhancement of nano-FTIR signals of a thin organic layer by exploiting polariton-resonant tip-substrate coupling and surface polariton illumination of the probing tip. When the molecular vibration matches the tip-substrate resonance, we achieve up to nearly one order of magnitude signal enhancement on a phonon-polaritonic quartz (c-SiO2) substrate, as compared to nano-FTIR spectra obtained on metal (Au) substrates, and up to two orders of magnitude when compared to the standard infrared spectroscopy substrate CaF2. Our results will be of critical importance for boosting nano-FTIR spectroscopy towards the routine detection of monolayers and single molecules.

Explore related subjects

Keep this discovery

Explore connections, maps & timelines

BibTeXRIS

Marta Autore, Lars Mester, Monika Goikoetxea, R. Hillenbrand. 2021-05-20. Substrate matters: Surface-polariton enhanced infrared nanospectroscopy of molecular vibrations. https://doi.org/10.1021/acs.nanolett.9b03257

Cite the original work for its findings. Save a collection to share your selection of sources.

KEEP EXPLORING

Related papers

Nonlinear Magneto-Optical Probing of Time-Reversal Symmetry Breaking

Solid-state harmonic generation provides a nonlinear probe of symmetries encoded in electronic wave functions. In the subgap and weak-injection regime, time reversal pairs the harmonic responses driven by fields of opposite ellipticity, strongly suppressing elliptical dichroism in time-reversal-symmetric crystals. We show that, in a magnetic crystal, spin-orbit coupling transfers time-reversal-symmetry breaking from the spin sector to the orbital wave functions and lifts this pairing through the geometric phases of the electric-dipole current. Semiconductor-Bloch-equation calculations for centrosymmetric bilayer Cr2Ge2Te6 predict pronounced third-harmonic elliptical dichroism that reverses with the magnetization. Under linearly polarized driving, SOC-induced geometric-phase accumulation generates a nonlinear transverse current and strongly enhances the harmonic rotation and ellipticity. These results identify the geometric phase as a key microscopic contribution to the nonlinear magneto-optical response. This work establishes helicity-resolved harmonic emission and nonlinear polarimetry as complementary probes of spin-orbit-coupled magnetic order.

physics.optics

Spatiotemporal topological phase transitions in photonic spacetime crystals

Topological phase transitions have played a central role in topological physics. However, such transitions have so far been restricted to spatial or temporal crystals. Here, we transcend this conventional framework and report, for the first time, spatiotemporal topological phase transitions in photonic spacetime crystals - structures that are periodically modulated in both space and time. In a genuine photonic spacetime crystal composed of a dynamically modulated transmission-line metamaterial, we theoretically propose and experimentally demonstrate complete spatiotemporal topological phase transitions, characterized by the closing and reopening of both energy and momentum band gaps, along with changes in spatiotemporal topological invariants and topological phases. Furthermore, we directly observe a spatiotemporal, topologically localized state that exhibits causality-governed excitation and robustness to spatiotemporal disorders. Our findings reveal the interplay among space, time, and topology, establishing a unified framework that provides a comprehensive picture of the emerging topological spacetime physics and opening new avenues for robust spatiotemporal topological wave manipulations.

physics.optics

High-Resolution Sensing via Quantum States Discrimination

High-resolution sensing plays a significant role in scientific research and industrial production, but the practical implementation is constrained by the physical mechanisms of the sensors. To address the critical limitation, we propose a high-resolution sensing approach based on quantum state discrimination. Distinct from conventional strategies, the proposed approach constructs measurement operators in the orthogonal complement space rather than eigenspace of the eigenstate, thereby notably improving the discriminability among quantum states. Moreover, the experimental results via an optical microcavity demonstrate a potential sensing resolution of 4 $\times$ 10\textsuperscript{-6} \degree C and 18 p$ε$ respectively for temperature and strain, and further verify the feasibility of simultaneous sensing of the two parameters. This work establishs a universal approach for high-resolution sensing, and may be extended to different sensing platforms across various application scenarios.

physics.optics