The ultrafast scattering dynamics of intersubband polaritons in dispersive cavities embedding GaAs/AlGaAs quantum wells are studied directly within their band structure using a noncollinear pump-probe geometry with phase-stable midinfrared pulses. Selective excitation of the lower polariton at a frequency of ∼25 THz and at a finite in-plane momentum k_{‖} leads to the emergence of a narrowband maximum in the probe reflectivity at k_{‖}=0. A quantum mechanical model identifies the underlying microscopic process as stimulated coherent polariton-polariton scattering. These results mark an important milestone toward quantum control and bosonic lasing in custom-tailored polaritonic systems in the mid and far infrared.
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http://dx.doi.org/10.1103/PhysRevLett.128.247401 | DOI Listing |
J Chem Theory Comput
June 2024
Department of Physics and Astronomy, University of Delaware, Newark, Delaware 19716, United States.
Developing theoretical frameworks for vibrational strong coupling (VSC) beyond the single-mode approximation is crucial for a comprehensive understanding of experiments with planar Fabry-Pérot cavities. Herein, a generalized cavity molecular dynamics (CavMD) scheme is developed to simulate VSC of a large ensemble of realistic molecules coupled to an arbitrary 1D or 2D photonic environment. This approach is built upon the Power-Zienau-Woolley Hamiltonian in the normal mode basis and uses a grid representation of the molecular ensembles to reduce the computational cost.
View Article and Find Full Text PDFNat Commun
April 2024
CAS Key Laboratory of Standardization and Measurement for Nanotechnology, National Center for Nanoscience and Technology, Beijing, 100190, P. R. China.
Exciton-polaritons (polaritons) resulting from the strong exciton-photon interaction stimulates the development of novel low-threshold coherent light sources to circumvent the ever-increasing energy demands of optical communications. Polaritons from bound states in the continuum (BICs) are promising for Bose-Einstein condensation owing to their theoretically infinite quality factors, which provide prolonged lifetimes and benefit the polariton accumulations. However, BIC polariton condensation remains limited to cryogenic temperatures ascribed to the small exciton binding energies of conventional material platforms.
View Article and Find Full Text PDFNat Commun
April 2023
Department of Electrical Engineering and Computer Science, Massachusetts Institute of Technology, Cambridge, MA, USA.
Hybrid perovskites have emerged as a promising material candidate for exciton-polariton (polariton) optoelectronics. Thermodynamically, low-threshold Bose-Einstein condensation requires efficient scattering to the polariton energy dispersion minimum, and many applications demand precise control of polariton interactions. Thus far, the primary mechanisms by which polaritons relax in perovskites remains unclear.
View Article and Find Full Text PDFNature
April 2023
Institut für Physikalische und Theoretische Chemie, Universität Würzburg, Würzburg, Germany.
Quantum states depend on the coordinates of all their constituent particles, with essential multi-particle correlations. Time-resolved laser spectroscopy is widely used to probe the energies and dynamics of excited particles and quasiparticles such as electrons and holes, excitons, plasmons, polaritons or phonons. However, nonlinear signals from single- and multiple-particle excitations are all present simultaneously and cannot be disentangled without a priori knowledge of the system.
View Article and Find Full Text PDFPhys Rev Lett
June 2022
Department of Physics, University of Regensburg, 93040 Regensburg, Germany.
The ultrafast scattering dynamics of intersubband polaritons in dispersive cavities embedding GaAs/AlGaAs quantum wells are studied directly within their band structure using a noncollinear pump-probe geometry with phase-stable midinfrared pulses. Selective excitation of the lower polariton at a frequency of ∼25 THz and at a finite in-plane momentum k_{‖} leads to the emergence of a narrowband maximum in the probe reflectivity at k_{‖}=0. A quantum mechanical model identifies the underlying microscopic process as stimulated coherent polariton-polariton scattering.
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