Bulletin of the American Physical Society
APS March Meeting 2020
Volume 65, Number 1
Monday–Friday, March 2–6, 2020; Denver, Colorado
Session A05: The Chemical Physics of Molecular Polaritons I. PhotophysicsFocus
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Sponsoring Units: DCP DCMP DPOLY Chair: Joel Yuen-Zhou, University of California, San Diego Room: 111 |
Monday, March 2, 2020 8:00AM - 8:36AM |
A05.00001: Assessing Polariton Amended Excited State Photophysics and Structure of Metalloporphyrins using Ultrafast and Nonlinear Optical Spectroscopy Invited Speaker: Aaron Rury The control of the photophysical and photochemical properties of molecules through truly quantum mechanisms remains an oustanding goal for the chemical physics community. The strong coupling of spatially confined photons to the electrons of molecules appears among the most promising quantum mechanisms test for molecular control. The formation of cavity polaritons through this strong coupling mechanism has been proposed to amend the excited state structure of molecules embedded in electromagnetic resonantors. Despite these proposals, definite experimental evidence of changes to the dynamics and structure of molecular cavity polaritons remain elusive. In this talk I present experimental results demonstrating the ways in which polariton formation amends the dynamics and structure of strongly cavity-coupled metalloporphyrin molecules. First, I examine how the strong coupling of photons in a nanoscale cavity to the Soret resonance of zinc tetraphenylporphyrin (ZnTPP) affects the competition between excited state absorption and fluorescence processes. I show polariton formation incerases the cross section of excited state absorption relative to stimulated emission. Second, I highlight ultrafast spectroscopic results demonstrating the control of energy gap laws via deterministic polariton formation. In particular, these results show the time scale of populating of an excited singlet state of ZnTPP can be controlled through changes to the Rabi splitting. Third, I propose nonlinear optical spectroscopic methods capable of directly assessing the ways the structure of a molecular excited state change in response to polariton formation. These results demonstrate the power of vibrational light scattering spectroscopies to not only assess structural changes central to the proposed control available through polariton formation, but also novel quantum optical phenomena polaritons may enable. |
Monday, March 2, 2020 8:36AM - 8:48AM |
A05.00002: Optical activity from exciton Aharonov-Bohm effect: a Floquet engineering
approach Kai Schwennicke We theoretically demonstrate that an originally achiral molecular system can exhibit nonzero circular dichroism (CD), through Floquet engineering, when it is driven with elliptically polarized light. More specifically, we consider an isotropic ensemble of small cyclic molecular aggregates in solution whose local low-frequency vibrational modes are driven by a continuous-wave infrared pump. We attribute the origin of the nonzero CD to time-reversal symmetry breaking due to an excitonic Aharonov-Bohm (AB) phase arising from laser-driving and coherent interchromophoric exciton hopping. The obtained Floquet-engineered excitonic AB phases are far more tunable than their analogous electronic AB phases in the nanoscale, highlighting a virtually unexplored potential that excitonic AB phases have in the coherent control of molecular processes and simultaneously introducing new analogues of magneto-optical effects in molecular systems which bypass the use of strong magnetic fields. |
Monday, March 2, 2020 8:48AM - 9:24AM |
A05.00003: Controlling Coherent Light-Matter Interactions in Semiconductors Invited Speaker: Hui Deng Light-matter interactions are at the heart of quantum electrodynamics and underpin modern photonic technologies. As we develop means to control the properties of light, matter and their interactions, intriguing new phenomena emerge. Using the mature, III-Arsenide semiconductor system, we build a designer cavity platform of polaritons 1. With it, we demonstrate a shot-noise limited polariton lasers with strong nonlinearities 2 and a Bardeen-Cooper-Schrieffer like polariton condensate 3. Coupling two trapped polariton condensates through both coherent tunneling and incoherent dissipation, we form a model system of rich nonlinear dynamics where new, equidistant frequency lines emerge due to limit cycle self-oscillations 4. Extension to larger arrays together with the flexibility to engineer fundamental properties of the polaritons may enable the discovery and understanding of new quantum many-body states. Using two-dimensional van der Waals semiconductors, we establish coherent light-matter coupling in a variety of photonic structures with unprecedented freedom to engineer both the optical modes and excitonic properties 5–7, which may enable new many-body phenomena and novel photonic device concepts. |
Monday, March 2, 2020 9:24AM - 9:36AM |
A05.00004: Topological polaritons and magneto-optical materials Sindhana Selvi Pannir Sivajothi, Joel Yuen-Zhou In recent years topological polaritons have been theoretically proposed and also observed in experiment. Our work aims to understand the fundamental features for a system to exhibit topological polaritons. We find that topological polaritonic states emerge in magneto-optical materials strongly coupled to surface plasmons in the presence of a magnetic field. In this particular system, we numerically demonstrate unidirectional edge modes. |
Monday, March 2, 2020 9:36AM - 9:48AM |
A05.00005: Quantum optics with molecules Claudiu Genes
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