Bulletin of the American Physical Society
APS March Meeting 2018
Volume 63, Number 1
Monday–Friday, March 5–9, 2018; Los Angeles, California
Session X02: Strong Light-matter Coupling and Enhanced Spectroscopy: Strong Coupling IIFocus
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Sponsoring Units: DCP DAMOP Chair: Jeffrey Owrutsky, Naval Research Lab Room: LACC 150B |
Friday, March 9, 2018 8:00AM - 8:36AM |
X02.00001: Hot Carrier Dynamics in Photoexcited Metal Nanostructures: Carrier Transport and Approaches to Photocatalysis Invited Speaker: Harry Atwater Excited electronic states in semiconductors and metals have the potential to alter the rate and selectivity of molecular reduction and oxidation reactions in photocatalysis. Doing so requires an accurate description and understanding of resonant optical absorption, excited carrier generation, relaxation and interfacial charge transfer processes, so as to understand the prospects for directing catalytic processes with optically generated excited carriers. Advances in theory and simulation of excited state carrier generation and transport processes will be discussed, as well as new experimental developments in optical design of resonant photocatalysts and photoelectrodes for solar fuel generators. |
Friday, March 9, 2018 8:36AM - 8:48AM |
X02.00002: Ab initio study of plasmon-induced direct hot-electron transfer at metal-acceptor interfaces Priyank Kumar, Tuomas Rossi, Martti Puska, David Norris Plasmon-induced hot-electron transfer at metal-molecule and metal-semiconductor interfaces is an important step in photocatalysis, photodetection and photovoltaics. The hot-electron transfer can occur via two mechanisms: (i) indirect transfer, where the hot electrons and holes are first produced in the metal nanostructure and eventually get transferred to the acceptor, (ii) direct transfer, where the plasmons decay by directly exciting an electron from the metal to the acceptor. Controlling and favoring the direct transfer process is crucial as one can bypass the electron-electron scattering step in the metal, thus avoiding energy losses. However, the atomic-level details and knowledge of the efficiency of this direct transfer process are missing. Using model metal-acceptor interfaces, we present an ab initio study based on time-dependent density functional theory (TDDFT) calculations to address this issue. We envision our computations to provide theoretical guidelines to design more efficient metal-molecule and metal-semiconductor interfaces. |
Friday, March 9, 2018 8:48AM - 9:00AM |
X02.00003: Optical Absorption of Materials Driven Far from Equilibrium by Lasers Bing Gu, Antonio Garzon, Ignacio Franco We propose a general theory for the optical absorption of matter driven far from equilibrium by lasers. Specifically, we envision a situation in which non-perturbative light drives a system out of equilibrium while a second weak probe quantifies its ability to absorb light across the electromagnetic spectrum. The interaction between matter and the driving pulse is treated exactly through a Floquet analysis, while the probe light is considered perturbatively. The procedure results in a generalization of the usual expressions for optical absorption to the non-equilibrium case. Through computations in model one-dimensional semiconductors, we unveil two striking phenomena that can reversibly be induced by non-resonant light of intermediate intensity (non-perturbative but non-ionizing). Specifically, we show that light can reversibly turn a semiconductor into a broadband absorber, and generate a strong absorption/stimulated emission band at arbitrarily low frequencies. This development offers a general approach to understand the emergent optical properties of materials dressed by the electric field of light and catalyze the design of laser-dressed materials. |
Friday, March 9, 2018 9:00AM - 9:36AM |
X02.00004: Cavity-Vibration Mixed States Invited Speaker: James Coe
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Friday, March 9, 2018 9:36AM - 9:48AM |
X02.00005: Nanoimaging and control of molecular vibrations through electromagnetically induced scattering reaching the strong coupling regime Eric Muller, Benjamin Pollard, Hans Bechtel, Ronen Adato, Hatice Altug, Markus Raschke Optical resonators, such as plasmonic nanoparticles and optical microcavities, have garnered significant attention recently as a way to enhance and modify the light-matter interaction. The long lifetimes of IR active molecular vibrations combined with the strongly subwavelength optical mode volumes of nanophotonic resonators offer an opportunity to observe novel phenomena through coupled multilevel systems with engineered light matter interactions and modification of vibrational excitation. |
Friday, March 9, 2018 9:48AM - 10:00AM |
X02.00006: Manipulating Molecules with Strong Coupling: Polariton-Enhanced Triplet Harvesting Andrew Musser, Daniel Polak, Rahul Jayaprakash, Kealan Fallon, Anastasia Leventis, John Anthony, Hugo Bronstein, David Lidzey, Jenny Clark A major focus in the study of organic exciton-polaritons has been the search for polariton condensation and lasing. However, their room-temperature stability and the large oscillator strengths of organic semiconductors offer the possibility for a wide range of further polaritonic effects. Indeed, within the strong coupling regime the upper and lower polariton states can be tuneably separated by as much as 100’s of meV from the parent exciton in these materials, enabling radical alteration of the energetic landscape. The effects of strong coupling can be profound, with reports of long-range energy transfer, altered chemical reactivity and work function modification. Theoretical work is now increasingly focused on the potential of strong coupling to manipulate electronic dynamics in the excited state. Here, we demonstrate for the first time the ability to manipulate the dynamics of singlet exciton fission using strong coupling. Within microcavities, we dramatically enhance the emission lifetime and increase delayed fluorescence by >75%, which we explain through a shift in the thermodynamic equilibrium between dark states in the exciton reservoir and the bright polaritons. |
Friday, March 9, 2018 10:00AM - 10:12AM |
X02.00007: Strong light-matter coupling using arrays of nanoantennas Mohammad Ramezani, Alexei Halpin, Antonio Fernandez-Dominguez, Johannes Feist, Quynh Le Van, Said Rahimzadeh-Kalaleh Rodriguez, Francisco Garcia Vidal, Jaime Gomez Rivas Metallic nanostructures have increasingly been applied as a platform for exploring the physics of strong-light matter coupling, through their ability to confine light leading to large local fields. Recent attention along this theme has been focused on molecular systems at room temperature, resulting in several exciting observations arising from the hybridization of photonic modes both with excitons and phonons to form quasi-particles known as polaritons. In this contribution we focus on strong-coupling between molecules and the resonances supported by periodic arrays of nanoantennas. These planar arrays define open cavities, with a dual benefit of broad tuneability and unique dispersions, and we will highlight recent work regarding polariton lasing from these structures. |
Friday, March 9, 2018 10:12AM - 10:24AM |
X02.00008: Polariton-assisted Singlet Fission in acene Aggregates Luis Martinez-Martinez, Matt Du, Raphael Ribeiro, Joel Yuen-Zhou The recent developments of nanostructures that can afford a strong confinement of electromagnetic fields have opened up avenues to explore different regimes of strong light-matter interaction. Under these, photonic and material degrees of freedom mix and give rise to hybrid entities usually known as polaritons. |
Friday, March 9, 2018 10:24AM - 10:36AM |
X02.00009: Multidimensional spectroscopy in optical cavities based on photon correlations Konstantin Dorfman, Shaul Mukamel Quantum electrodynamical effects in microcavities provide a powerful tool for studying quantum effects in matter which include the manipulation of chemical reactions rates and outcomes. These can be described by the Jaynes-Cummings model which represents a two-level atom interacting with quantized cavity modes and is a pillar of modern quantum optics. The time dependence in matter-cavity coupling resembles molecular dynamics and is a cornerstone of the studies of molecular dynamics in cavities. Here we show that the response of a two-level atom to the time-dependent coupling to a single cavity mode can be monitored by a new type of time-and-frequency resolved photon correlation measurements of spontaneous emission into noncavity modes. This novel multidimensional optical spectroscopy technique is based on single photon counting and can monitor the atom-cavity dressed state population and coherence dynamics for a given cavity photon number. Simultaneous time-and-frequency gating allows to precisely determine the hybrid state of molecule plus cavity without interfering with the cavity photon statistics. |
Friday, March 9, 2018 10:36AM - 10:48AM |
X02.00010: Organic polariton devices Stephane Kena-Cohen, Fabio Barachati, Elad Eizner We will describe recent efforts to engineer polariton light-emitters, photodiodes and tunable light sources. We will present a critical look at the role of polaritonic effects in charge transport, nonlinear behaviour, and other phenomena. In addition, we will describe our efforts and those of other groups to re-order excited states using organic microcavities in order to modify dynamics in a way that could be useful for devices. |
Friday, March 9, 2018 10:48AM - 11:00AM |
X02.00011: Photocurrent Enhancement by a Polariton Condensate David Myers, Burcu Ozden, Mark Steger, Loren Pfeiffer, K West, David Snoke We show that a condensate of exciton-polaritons greatly increases the current through a GaAs/AlAs device. These polaritons are bosons that result from coupling trapped microcavity photons with quantum well excitons. This effectively results in photons that have been dressed with mass and repulsive interactions, allowing them to undergo Bose-Einstein condensation. We fabricated ≈100 μm × 100 μm square pillars to confine the polaritons [1], and then drove in-plane current through the polariton region by placing contacts on opposite sides of the pillars. The use of identical contacts on both sides resulted in an n-i-n structure, allowing injection of only free electrons. In addition to current enhancement, we also observed stimulated injection of free carriers into polariton condensates trapped in these pillars, resulting in greatly increased polariton density. |
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