Polariton pulses-transient light-matter hybrid excitations-traveling through anisotropic media can lead to unusual optical phenomena in space and time. However, studying these pulses presents challenges with their anisotropic, ultrafast, and nanoscale field variations. Here, we demonstrate the creation, observation, and control of polariton pulses, with in-plane hyperbolic dispersion, on anisotropic crystal surfaces by using a time-resolved nanoimaging technique and our developed high-dimensional data processing. We capture and analyze movies of distinctive pulse spatiotemporal dynamics, including curved ultraslow energy flow trajectories, anisotropic dissipation, and dynamical misalignment between phase and group velocities. Our approach enables analysis of polariton pulses in the wave vector time domain, demonstrating a time-domain polaritonic topological transition from lenticular to hyperbolic dispersion contours and the ability to study the polariton-induced time-varying optical forces. Our findings promise to facilitate the study of diverse space-time phenomena at extreme scales and drive advances in ultrafast nanoimaging.
Download full-text PDF |
Source |
---|---|
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC10456838 | PMC |
http://dx.doi.org/10.1126/sciadv.adi4407 | DOI Listing |
Nano Lett
January 2025
Regensburg Center for Ultrafast Nanoscopy (RUN) and Department of Physics, University of Regensburg, 93040 Regensburg, Germany.
Detecting electromagnetic radiation scattered from a tip-sample junction has enabled overcoming the diffraction limit and started the flourishing field of polariton nanoimaging. However, most techniques only resolve amplitude and relative phase of the scattered radiation. Here, we utilize field-resolved detection of ultrashort scattered pulses to map the dynamics of surface polaritons in both space and time.
View Article and Find Full Text PDFJ Chem Theory Comput
December 2024
Max Planck Institute for the Structure and Dynamics of Matter, Luruper Ch 149, Hamburg 22761, Germany.
High-harmonic generation (HHG) is a nonlinear process in which a material sample is irradiated by intense laser pulses, causing the emission of high harmonics of incident light. HHG has historically been explained by theories employing a classical electromagnetic field, successfully capturing its spectral and temporal characteristics. However, recent research indicates that quantum-optical effects naturally exist or can be artificially induced in HHG, such as entanglement between emitted harmonics.
View Article and Find Full Text PDFNanophotonics
June 2024
Nanoscience Center and Department of Chemistry, University of Jyväskylä, P.O. Box 35, 40014 Jyväskylä, Finland.
Placing a material inside an optical cavity can enhance transport of excitation energy by hybridizing excitons with confined light modes into polaritons, which have a dispersion that provides these light-matter quasi-particles with low effective masses and very high group velocities. While in experiments, polariton propagation is typically initiated with laser pulses, tuned to be resonant either with the polaritonic branches that are delocalized over many molecules, or with an uncoupled higher-energy electronic excited state that is localized on a single molecule, practical implementations of polariton-mediated exciton transport into devices would require operation under low-intensity incoherent light conditions. Here, we propose to initiate polaritonic exciton transport with a photo-acid, which upon absorption of a photon in a spectral range not strongly reflected by the cavity mirrors, undergoes ultra-fast excited-state proton transfer into a red-shifted excited-state photo-product that can couple collectively with a large number of suitable dye molecules to the modes of the cavity.
View Article and Find Full Text PDFNanophotonics
May 2024
Pacific Northwest National Laboratory, Physical Sciences Division, Richland, WA 99354, USA.
J Chem Phys
November 2024
Department of Engineering and Applied Sciences, Sophia University, 7-1 Kioi-cho, Chiyoda, Tokyo 102-8554, Japan.
Metal halide perovskite materials (MHPs) are promising for several applications due to their exceptional properties. Understanding excitonic properties is essential for exploiting these materials. For this purpose, we focus on CsPbBr3 single crystals, which have higher crystal quality, are more stable, and have no Rashba effect at low temperatures compared to other 3D MHPs.
View Article and Find Full Text PDFEnter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!