Semiclassical quantization rules and numerical calculations are applied to study polariton modes of materials whose permittivity tensor has principal values of opposite sign (so-called hyperbolic materials). The spectra of volume- and surface-confined polaritons are computed for spheroidal nanogranules of hexagonal boron nitride, a natural hyperbolic crystal. The field distribution created by polaritons excited by an external dipole source is predicted to exhibit raylike patterns due to classical periodic orbits. Near-field infrared imaging and Purcell-factor measurements are suggested to test these predictions.
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http://dx.doi.org/10.1021/acs.nanolett.5b00814 | DOI Listing |
J Chem Theory Comput
January 2025
Department of Chemistry, Brandeis University, 415 South Street, Waltham, Massachusetts 02453, United States.
The photocatalytic efficiency of materials such as graphene and noble metal nanoclusters depends on their plasmon lifetimes. Plasmon dephasing and decay in these materials is thought to occur on ultrafast time scales, ranging from a few femtoseconds to hundreds of femtoseconds and longer. Here we focus on understanding the dephasing and decay pathways of excited states in small lithium and silver clusters and in plasmonic states of the π-conjugated molecule anthracene, providing insights that are crucial for interpreting optical properties and photophysics.
View Article and Find Full Text PDFJ Chem Phys
January 2025
Department of Chemistry, University of Rochester, Rochester, New York 14627, USA.
We outline two general theoretical techniques to simulate polariton quantum dynamics and optical spectra under the collective coupling regimes described by a Holstein-Tavis-Cummings (HTC) model Hamiltonian. The first one takes advantage of sparsity of the HTC Hamiltonian, which allows one to reduce the cost of acting polariton Hamiltonian onto a state vector to the linear order of the number of states, instead of the quadratic order. The second one is applying the well-known Chebyshev series expansion approach for quantum dynamics propagation and to simulate the polariton dynamics in the HTC system; this approach allows us to use a much larger time step for propagation and only requires a few recursive operations of the polariton Hamiltonian acting on state vectors.
View Article and Find Full Text PDFJ Chem Theory Comput
January 2025
Department of Theoretical Physics, University of Debrecen, P.O. Box 400, Debrecen H-4002, Hungary.
The coupling of matter to the quantized electromagnetic field of a plasmonic or optical cavity can be harnessed to modify and control chemical and physical properties of molecules. In optical cavities, a term known as the dipole self-energy (DSE) appears in the Hamiltonian to ensure gauge invariance. The aim of this work is twofold.
View Article and Find Full Text PDFNat Commun
December 2024
Department of Physics and Astronomy, Seoul National University, Seoul, 08826, Korea.
Fermi polarons are emerging quasiparticles when a bosonic impurity immersed in a fermionic bath. Depending on the boson-fermion interaction strength, the Fermi-polaron resonances exhibit either attractive or repulsive interactions, which impose further experimental challenges on understanding the subtle light-driven dynamics. Here, we report the light-driven dynamics of attractive and repulsive Fermi polarons in monolayer WSe devices.
View Article and Find Full Text PDFNanomaterials (Basel)
December 2024
Theoretical Physical Chemistry, UR MOLSYS, University of Liege, B4000 Liège, Belgium.
Dynamical symmetries, time-dependent operators that almost commute with the Hamiltonian, extend the role of ordinary symmetries. Motivated by progress in quantum technologies, we illustrate a practical algebraic approach to computing such time-dependent operators. Explicitly we expand them as a linear combination of time-independent operators with time-dependent coefficients.
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