Bulletin of the American Physical Society
APS March Meeting 2020
Volume 65, Number 1
Monday–Friday, March 2–6, 2020; Denver, Colorado
Session L05: The Chemical Physics of Molecular Polaritons V. Plasmonic CavitiesFocus
|
Hide Abstracts |
Sponsoring Units: DCP DCMP DPOLY Room: 111 |
Wednesday, March 4, 2020 8:00AM - 8:36AM |
L05.00001: Manipulating nonadiabatic conical intersection dynamics by optical cavities Invited Speaker: Shaul Mukamel Optical cavities hold great promise to manipulate and control the photochemistry of molecules. We demonstrate how molecular photochemical processes can be manipulated by strong light-matter coupling. For a molecule with an inherent conical intersection, optical cavities can induce significant changes in the nonadiabatic dynamics by either splitting the pristine conical intersections into two novel polaritonic conical intersections or by creating light-induced avoided crossings in the polaritonic surfaces. This is demonstrated by exact real-time quantum dynamics simulations of a three-state two-mode model of pyrazine strongly coupled to a single cavity photon mode. We further explore the effects of external environments through dissipative polaritonic dynamics computed using the hierarchical equation of motion method. We find that cavity-controlled photochemistry can be immune to external environments. We demonstrate that the polariton-induced changes in the dynamics can be monitored by transient absorption spectroscopy. |
Wednesday, March 4, 2020 8:36AM - 8:48AM |
L05.00002: Effect of Stokes shift on molecular polariton dynamics Jussi Toppari, Gerrit Groenhof, Tero T Heikkilä Strong coupling between molecules and confined light, like surface plasmon polaritons (SPP) or cavity photons (CP), leads to a formation of polariton states manifested by a Rabi split in the absorption spectrum. This changes the energy landscape of the molecules and can alter their chemical behavior. However, the Stokes shift of the molecule can play an essential role here. |
Wednesday, March 4, 2020 8:48AM - 9:00AM |
L05.00003: hoton emission properties of polariton states of rhodamine dyes in 2D plasmonic cavity Oleksiy Roslyak, Eric Bittner, Andrei Piryatinski Using our generalization of the Dicke model for quantum emitters coupled to surface plasmon modes, we have predicted a reach phase diagram of plasmon-exciton-polartion states depending on the interaction strengths between the surface plasmon modes and quantum emitters.1 For the purpose of practical implications, we study R6G rhodamine dye quantum emitters placed in a plasmonic cavity. The cavity is constituted from metal nanoparticles forming a rectangular 2D lattice. CDA analysis reveals intricate combinations of a bright local surface plasmon resonance (LSPR) on each nanoparticle and dark diffractive orders present in periodic structures resulting in a sharp Fano shaped surface lattice resonance (SLR). Concentration dependent coupling to R6G simulated via effective dielectric medium approach at CDA and RCWA levels. Extracted coupling rates between the SLR and the rhodamine dyes allow us to map the problem on the Dicke Hamiltonian. The polariton branches of the Hamiltonian are evaluated and subsequent analysis of the associated state photon emission properties is performed. |
Wednesday, March 4, 2020 9:00AM - 9:36AM |
L05.00004: Bose-Einstein Condensation and stimulated thermalization of polaritons in plasmonic lattices Invited Speaker: Paivi Torma
|
Wednesday, March 4, 2020 9:36AM - 9:48AM |
L05.00005: Tailoring weak-to-strong coupling of a plasmonic-photonic cavity Feng Pan, Randall H. Goldsmith Control of light–matter interactions is important to a number of advances in quantum communication, information and sensing. Tailoring coupling strength relative to loss rates is central to exert control over the interactions. Recently we have demonstrated we could pin down a high dynamic range of system parameters in a coupled plasmonic-photonic cavity. Embedding the coupled cavity with an index-matching polymer matrix allows plasmonic and photonic modes to be largely overlapped and thus lifts up g to the same order of magnitude as dominant nonradiative loss rate, potentially leading to a strongly coupled cavity. After the coupled cavity is embedded by polydimethylsiloxane (PDMS). Plasmonic resonance of a gold nanorod (AuNR) is red-shifted due to change of local dielectric environment around the AuNR. Decreasing the aspect ratio blue-shifts its plasmon resonance back to our spectral window and then we observe a splitting spectral feature that signifies strong coupling. This demonstration provides an avenue for tailoring weak-to-strong coupling, which foreshadows the potential of entangling multiple plasmonic systems through photonic mode for protection against decoherence in quantum communication. |
Wednesday, March 4, 2020 9:48AM - 10:00AM |
L05.00006: Strong coupling beyond the light-line Kishan Menghrajani, William L Barnes Many experiments on strong coupling of molecules make use of metal-clad microcavities. Coupling is usually investigated between the excitonic or vibronic molecular resonance (as appropriate) and the lowest order cavity mode. However, metal-clad microcavities also support a coupled surface plasmon mode, something that appears to have been ignored in previous work, probably because it exists beyond the light-line. Here we show that this coupled plasmon mode also interacts with molecular resonances to produce hybrid polariton modes. |
Wednesday, March 4, 2020 10:00AM - 10:36AM |
L05.00007: Modified excited states dynamics in the nanoparticle plasmon – molecular exciton hybrids under strong coupling regime Invited Speaker: Timur Shegai Strong light-matter interactions in microcavities have been long known to provide means to alter optical and nonlinear properties of the coupled system. As a result of this interaction, one typically observes the emergence of new polaritonic eigenstates. These states are of hybrid nature and possess both light and matter characteristics, which is reflected in vacuum Rabi splitting, observed in the absorption or transmission spectra. Because of the hybrid nature of these states, the excited state temporal dynamics can be significantly altered in comparison to the uncoupled system dynamics. This, in turn, can have profound effects on the emission and photochemical processes. |
Wednesday, March 4, 2020 10:36AM - 10:48AM |
L05.00008: Cavity Induced Non-adiabatic Effects and Modifications of the Spin-orbit Coupling Dominik Sidler, Michael Ruggenthaler, Heiko Appel, Angel Rubio A numerically exact diagonalisation of the non-relativistic Pauli-Fierz Hamiltonian is performed for quantized three-body problems coupled to one cavity mode in 3D. The resulting 10-dimensional setup can be transformed into an effectively five dimensional problem, which is fully diagonalisable with state-of-the-art computers. This allows to investigate polaritonic effects for real systems (e.g. He or HD+) with high accuracy, potentially giving access to cavity induced non-adiabatic effects. Modifications of the fine-structure arising from the coupling to a quantized cavity mode can be treated perturbatively. |
Follow Us |
Engage
Become an APS Member |
My APS
Renew Membership |
Information for |
About APSThe American Physical Society (APS) is a non-profit membership organization working to advance the knowledge of physics. |
© 2024 American Physical Society
| All rights reserved | Terms of Use
| Contact Us
Headquarters
1 Physics Ellipse, College Park, MD 20740-3844
(301) 209-3200
Editorial Office
100 Motor Pkwy, Suite 110, Hauppauge, NY 11788
(631) 591-4000
Office of Public Affairs
529 14th St NW, Suite 1050, Washington, D.C. 20045-2001
(202) 662-8700