skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.

Explore Research Products in the PAR
It may take a few hours for recently added research products to appear in PAR search results.


Title: Tip‐Enhanced Imaging and Control of Infrared Strong Light‐Matter Interaction
Optical antenna resonators enable control of light‐matter interactions on the nano‐scale via electron–photon hybrid states in strong coupling. Specifically, mid‐infrared (MIR) nano‐antennas coupled to saturable intersubband transitions in multi‐quantum‐well (MQW) semiconductor heterostructures allow for the coupling strength to be tuned through antenna resonance and field intensity. Here, tip‐enhanced nano‐scale variation of antenna‐MQW coupling across the antenna is demonstrated, with a spatially‐dependent coupling strength varying from 73 (strong coupling) to 24 (weak coupling). This behavior is modeled based on the spatially dependent local constructive and destructive interference between tip and antenna fields. Using a quantum‐mechanical density‐matrix model of the MQW system with its designed values of transition dipole moment, doping density, and population decay time, the picosecond IR pulse coupling to intersubband transitions and the associated tip induced strong‐field saturation effects are described. These results present a new regime of nonlinear IR light‐matter control based on the dynamic manipulation of quantum hybrid states on the nanoscale and in the infrared, with a perspective regarding extension to molecular vibrations.  more » « less
Award ID(s):
2108009
PAR ID:
10538266
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ; ; ;
Publisher / Repository:
Wiley
Date Published:
Journal Name:
Laser & Photonics Reviews
ISSN:
1863-8880
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. ; ; ; ; ; ; ; (, Science Advances)
    Optical cavities can enhance and control light-matter interactions. This level of control has recently been extended to the nanoscale with single emitter strong coupling even at room temperature using plasmonic nanostructures. However, emitters in static geometries, limit the ability to tune the coupling strength or to couple different emitters to the same cavity. Here, we present tip-enhanced strong coupling (TESC) with a nanocavity formed between a scanning plasmonic antenna tip and the substrate. By reversibly and dynamically addressing single quantum dots, we observe mode splitting up to 160 meV and anticrossing over a detuning range of ~100 meV, and with subnanometer precision over the deep subdiffraction-limited mode volume. Thus, TESC enables previously inaccessible control over emitter-nanocavity coupling and mode volume based on near-field microscopy. This opens pathways to induce, probe, and control single-emitter plasmon hybrid quantum states for applications from optoelectronics to quantum information science at room temperature. 
    more » « less
  2. ; ; ; ; ; ; ; ; ; ; et al (, Physical Review Letters)
    Exciton-polaritons confined in plasmonic cavities are hybridized light-matter quasiparticles, with distinct optical characteristics compared to plasmons and excitons alone. Here, we demonstrate the electric tunability of a single polaritonic quantum dot operating at room temperature in electric-field tip-enhanced strong coupling spectroscopy. For a single quantum dot in the nanoplasmonic tip cavity with variable dc local electric field, we dynamically control the Rabi frequency with the corresponding polariton emission, crossing weak to strong coupling. We model the observed behaviors based on the quantum confined Stark effect in the strong coupling regime. 
    more » « less
  3. ; ; ; ; ; ; ; (, Optics Letters)
    The advent of layered materials has unveiled new opportunities for tailoring electromagnetic waves at the subwavelength scale, particularly through the study of polaritons, a hybrid light–matter excitation. In this context, twist-optics, which investigates the optical properties of twisted stacks of van der Waals (vdW) layered specimens, has emerged as a powerful tool. Here, we explore the tunability of phonon polaritons in α-V2O5via interlayer twisting using scanning nano-infrared (IR) imaging. We show that the polaritonic response can be finely adjusted by varying their interlayer electromagnetic coupling, allowing for precise control over the propagation direction and phase transition from open unidirectional iso-frequency contours to closed elliptic geometries. Our experimental results, in conjugate with theoretical modeling, reveal the mechanisms underpinning this tunability, highlighting the role of twist-induced nano-light modifications for advanced nanophotonic control at the nanoscale. 
    more » « less
  4. ; ; ; ; ; ; ; ; (, Proc. SPIE 12009, Quantum Sensing and Nano Electronics and Photonics XVIII)
    Razeghi, Manijeh; Khodaparast, Giti A.; Vitiello, Miriam S. (Ed.)
    Band structure, strain, and polarization engineering of nitride heterostructures open unparalleled opportunities for quantum sensing in the infrared. Intersubband absorption and photoluminescence are employed to correlate structure with optical properties of nonpolar strain-balanced InGaN/AlGaN nanostructures grown by molecular-beam epitaxy. Mid-infrared intersubband transitions in m-plane (In)AlxGa1-xN/In0.16Ga0.84N (0.19x0.3) multi-quantum wells were observed for the first time in the range of 3.4-5.1 μm (244-360 meV). Direct and attenuated total-reflection infrared absorption measurements are interpreted using structural information revealed by high-resolution x-ray diffraction and transmission electron microanalysis. The experimental intersubband energies are better reproduced by calculations using the local-density approximation than the Hartree-Fock approximation for the exchange-correlation correction. The effect of charge density, quantum well width, and barrier alloy composition on the intersubband transition energy was examined to evaluate the potential of this material for practical infrared applications. Temperature-dependent continuous-wave and time-resolved photoluminescence (TRPL) measurements are also investigated to probe carrier localization and recombination in m-plane InGaN/AlGaN quantum wells. Average localization depths of 21 meV and 40 meV were estimated for the undoped and doped structures, respectively. Using TRPL, dual localization centers were identified in undoped structures, while a single type of localization centers was found in doped structures. At 2 K, a fast decay time of approximately 0.3ns was measured for both undoped and doped structures, while a longer decay time of 2.2 ns was found only for the undoped sample. TRPL in magnetic field was explored to examine the effect of doping sheets on carrier dynamics. 
    more » « less
  5. ; ; ; ; ; (, Chemical Reviews)
    When molecules are coupled to an optical cavity, new light–matter hybrid states, so-called polaritons, are formed due to quantum light–matter interactions. With the experimental demonstrations of modifying chemical reactivities by forming polaritons under strong light–matter interactions, theorists have been encouraged to develop new methods to simulate these systems and discover new strategies to tune and control reactions. This review summarizes some of these exciting theoretical advances in polariton chemistry, in methods ranging from the fundamental framework to computational techniques and applications spanning from photochemistry to vibrational strong coupling. Even though the theory of quantum light–matter interactions goes back to the midtwentieth century, the gaps in the knowledge of molecular quantum electrodynamics (QED) have only recently been filled. We review recent advances made in resolving gauge ambiguities, the correct form of different QED Hamiltonians under different gauges, and their connections to various quantum optics models. Then, we review recently developed ab initio QED approaches which can accurately describe polariton states in a realistic molecule–cavity hybrid system. We then discuss applications using these method advancements. We review advancements in polariton photochemistry where the cavity is made resonant to electronic transitions to control molecular nonadiabatic excited state dynamics and enable new photochemical reactivities. When the cavity resonance is tuned to the molecular vibrations instead, ground-state chemical reaction modifications have been demonstrated experimentally, though its mechanistic principle remains unclear. We present some recent theoretical progress in resolving this mystery. Finally, we review the recent advances in understanding the collective coupling regime between light and matter, where many molecules can collectively couple to a single cavity mode or many cavity modes. We also lay out the current challenges in theory to explain the observed experimental results. We hope that this review will serve as a useful document for anyone who wants to become familiar with the context of polariton chemistry and molecular cavity QED and thus significantly benefit the entire community. 
    more » « less
  • Citation Formats
  • MLA
  • APA
  • Chicago
  • BibTeX
  • Text Encoded Conversion
  • XML
  • Save / Share this Record
  • Send to Email