相关论文: Ultrafast dynamics of CN radical reactions with ch…
Molecular polaritons, hybrid light-matter states resulting from strong cavity coupling of optical transitions, may provide a new route to guide chemical reactions. However, demonstrations of cavity-modified reactivity in clean benchmark…
Polaritons - hybrid light-matter states formed from the strong coupling of a bright molecular transition with a confined photonic mode - may offer new opportunities for optical control of molecular behavior. Vibrational strong coupling…
In vibrational strong coupling (VSC), molecular vibrations strongly interact with the modes of an optical cavity to form hybrid light-matter states known as vibrational polaritons. Experiments show that the kinetics of thermally activated…
Under vibrational strong coupling (VSC), the formation of molecular polaritons may significantly modify the photo-induced or thermal properties of molecules. In an effort to understand these intriguing modifications, both experimental and…
In this thesis, we use classical, semi-classical and quantum-mechanical methods to simulate chemical reaction dynamics inside of an optical cavity. Within such a cavity, by selectively coupling vibrational modes of the reactants to the…
Vibrational strong coupling (VSC) provides a novel means to modify chemical reactions and energy transfer pathways. To efficiently model chemical dynamics under VSC in the collective regime, herein a hybrid quantum mechanical/molecular…
Recent experiments have observed that the chemical and photophysical properties of molecules can be modified inside an optical Fabry-Perot microcavity under collective vibrational strong coupling (VSC) conditions, and such modification is…
In this paper we develop quantum dynamical methods capable of treating the dynamics of chemically reacting systems in an optical cavity in the vibrationally strong-coupling (VSC) limit at finite temperatures and in the presence of a…
For a small fraction of hot CO2 molecules immersed in a liquid-phase CO2 thermal bath, classical cavity molecular dynamics simulations show that forming collective vibrational strong coupling (VSC) between the C=O asymmetric stretch of CO2…
There is growing interest in using strongly coupled organic microcavities to tune molecular dynamics, including the electronic and vibrational properties of molecules. However, very little attention has been paid to the utility of cavity…
We introduce a prototypical model for cavity polaritonic control of ultracold photochemistry by considering the resonant vibrational strong coupling of a rubidium dimer to a terahertz cavity. We demonstrate that at avoided crossings between…
Polaritons have gained significant attention for the tantalizing possibility of modifying chemical properties and dynamics by coupling molecules to resonant cavity modes to create hybrid light-matter quantum states. Herein, we implement the…
Recent experiments showed that the chemical reaction rate is modified, either increased or decreased, by strongly coupling a nuclear vibration mode to the single mode of an optical cavity. Herein we investigate how the rate of an…
In the regime of ensemble vibrational strong coupling (VSC), a macroscopic number $N$ of molecular transitions couple to each resonant cavity mode, yielding two hybrid light-matter (polariton) modes, and a reservoir of $N-1$ dark states…
Recent reports suggest that chemical reaction rates can change when reactants are placed inside an optical cavity. These effects have been attributed to the hybridization of molecular vibrational modes with cavity modes into polaritons, but…
We simulate vibrational strong (VSC) and ultrastrong coupling (V-USC) for liquid water with classical molecular dynamics simulations. When the cavity modes are resonantly coupled to the O-H stretch mode of liquid water, the infrared…
The concept of modifying molecular dynamics in strongly coupled exciton-polariton systems is an emerging topic in photonics due to its potential to produce customized chemical systems with tailored photophysical properties. However, before…
Manipulation of chemical reactivity often involves changing reagents or environmental conditions. Alternatively, strong coupling between light and matter offers a way to tunably hybridize their physicochemical properties and thereby change…
We introduce a theory of chemical equilibrium in optical microcavities, which allows us to relate equilibrium reaction quotients in different electromagnetic environments. Our theory shows that in planar microcavities under strong coupling…
Vibrational control (VC) of photochemistry through the optical stimulation of structural dynamics is a nascent concept only recently demonstrated for model molecules in solution. Extending VC to state-of-the-art materials may lead to new…