Bulletin of the American Physical Society
APS March Meeting 2021
Volume 66, Number 1
Monday–Friday, March 15–19, 2021; Virtual; Time Zone: Central Daylight Time, USA
Session M03: Ab-initio studies and novel effects of strong light-matter coupling in molecular, two-dimensional and solid-state systemsInvited Live
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Sponsoring Units: DCP DCMP Chair: Johannes Flick, Simons Foundation |
Wednesday, March 17, 2021 11:30AM - 11:54AM Live |
M03.00001: Insights on Photochemical Processes in the Strong Coupling Regime by Atomistic Simulations Invited Speaker: Stefano Corni Electronic excitations in molecules can be strongly coupled to electromagnetic modes of resonant cavities. The properties of the resulting hybrid states (polaritons) are different than those of the original electronic states. In particular, the resulting photochemistry depends on the features of the excited molecular states, and can therefore be modified by entering the strong coupling regime. As such, strong coupling is emerging as an elegant tool to manipulate the photochemistry (or rather the polaritonic chemistry) of molecules, elegant in that it is not relying on engineering of the molecule or of the solvent. In collaboration with the group of G. Granucci and M. Persico, we have developed an atomistic computational methodology [1] that extends to polaritonic chemistry a well-established semiclassical approach developed for photochemical processes [2]. We have applied it to azobenzene photoisomerization with a fully atomistic description of the molecule and of the surrounding environment to investigate how the mechanism and the yield of the reaction change entering the strong coupling regime [3,4]. The resulting picture is that of a complicated mechanism, where the modification of excited state lifetimes and effectiveness of vibrational energy redistribution play prominent roles [4]. Such mechanism could hardly be imagined a priori or on the basis of simplified theoretical models, showing the need of realistic simulations as a tool to discover and rationalize polaritonic chemistry mechanistic patterns to inspire experiments and further theoretical modeling. |
Wednesday, March 17, 2021 11:54AM - 12:30PM Live |
M03.00002: Coupled cluster theory for molecular polaritons Invited Speaker: Henrik Koch I will present our recently developed ab initio correlated approach to study molecules that interact strongly with quantum fields in an optical cavity. Quantum electrodynamics coupled cluster theory (QED-CC)1 provides a nonperturbative description of cavity-induced effects in ground and excited states. Using this theory, we show how quantum fields can be used to manipulate charge transfer and photochemical properties of molecules. We propose a strategy to lift electronic degeneracies and induce modifications in the ground-state potential energy surface close to a conical intersection. Cavity-induced modulation of intermolecular interactions are also discussed.2 |
Wednesday, March 17, 2021 12:30PM - 12:54PM Live |
M03.00003: Towards a detailed understanding of strong light-matter coupling effects Invited Speaker: Michael Ruggenthaler In the last decade a host of seminal experimental results have demonstrated that molecules and solids can be modified and controlled by coupling strongly to the electromagentic field of an optical cavity. Many of the observed effects are not well understood and the common models of strong light-matter coupling lead to contradictory conclusions. It therefore becomes desirable to have first-principles approaches to strong light-matter coupling in order to obtain a so far elusive detailed understanding of photon-modified matter properties. |
Wednesday, March 17, 2021 12:54PM - 1:30PM Live |
M03.00004: Co-operative Vibrational Strong Coupling: A New Route to Control Chemical Reactions Invited Speaker: Jino George Recently, vibrational strong coupling was used to control chemical reactions very preciously by targeting a vibrational state.[1] However, this process is limited to molecules having very strong vibrational bands that can undergo strong coupling. Here, we show an efficient way of controlling chemical reactions by co-operative vibrational strong coupling (Co-VSC).[2] This is specifically achieved by choosing a solvent that has a matching vibrational band to the reactant molecule responsible for the reaction. Coupling the bulk solvent gives very high Rabi splitting that reshuffles the energy of the reacting species. We catalysed a simple ester hydrolysis process by Co-VSC of C=O band of the ester (reactant) and ethyl acetate (solvent) in a flow cell Fabry-Perot cavity. This results in the dropping of the enthalpy and entropy of activation of the hydrolysis reaction. In another attempt, large biomolecules such as alpha-chymotrypsin is coupled to the vacuum field via Co-VSC of water.[3] In this case, we improved the enzyme catalysis process and found that cavity coupling can bring a competitive enhancement in the reaction. High sensitivity with cavity tuning and increase in the reaction rate with increasing coupling strength are the two important features of cavity catalysis. This is purely an unconventional way of controlling chemical reactions, that will have direct application in chemistry. |
Wednesday, March 17, 2021 1:30PM - 2:06PM Live |
M03.00005: Theory of collective cavity dynamics for cold chemistry and materials science Invited Speaker: Guido Pupillo Strong light-matter interactions are playing an increasingly crucial role in the understanding and engineering of new states of matter with relevance to the fields of quantum optics, solid state physics, chemistry and materials science. In this talk we focus on collective light matter interactions in the limit of vanishingly small photon numbers: Coupling matter to the vacuum electromagnetic field of a cavity – i.e. passively – can lead to permanent changes in the material due to the combined effects of vacuum hybridization, long-range cavity-mediated and direct couplings between material constituents. Examples of modified properties of strongly coupled systems, such as charge and energy transport, and chemical reactivity will be given to illustrate the potential of polaritonic states for molecular and material sciences. |
Wednesday, March 17, 2021 2:06PM - 2:30PM Live |
M03.00006: Non-thermal pathways to non-equilibrium control of correlated quantum materials Invited Speaker: Martin Claassen Leveraging coherent light-matter interaction in solids is a promising new direction towards control and functionalization of quantum materials, to potentially realize regimes inaccessible in equilibrium and stabilize new or useful states of matter. With time-resolved experiments taking rapid strides in the transient control of single-particle properties, a key question concerns the induction of many-body states far from equilibrium. In this talk, I will discuss avenues and challenges in how tailored light fields can provide a non-thermal handle to manipulate, induce and probe novel electronic or magnetic phases in strongly correlated materials. We will show how driving the strongly spin-orbit coupled proximal Kitaev magnet α-RuCl3 with light or THz radiation can give rise to a ligand-mediated magneto-electric effect and nudge the material towards the elusive Kitaev quantum spin liquid, with the transient competition of magnetic orders observable via pump-probe spectroscopy. I will then argue that heating and time scales of coherent manipulation can be understood in a flow renormalization framework for driven systems, in which dynamical regimes at intermediate times are represented as unstable fixed points of the flow, establishing a new tool to study long-lived prethermal quantum phases. |
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