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Enes Suyabatmaz

Publications and source records attributed to Enes Suyabatmaz.

3 recordsLinked to original sources

Polyatomic Thermal Radiative Dissociation in Microcavities

Blackbody infrared radiative dissociation (BIRD) activates molecules through successive absorption of ambient thermal photons until the internal energy reaches a dissociation threshold. Because these radiative transition rates depend on the electromagnetic density of states (DOS), structured infrared environments provide a route to control thermal unimolecular dissociation. Here we develop a state-resolved master-equation framework for polyatomic BIRD in a planar Au/MgO multilayer cavity, where the reactive cluster $\mathrm{(H_2O)_2Cl^-}$ is studied. The cavity modifies the kinetics through the DOS sampled by anharmonic fundamental, overtone, and combination transitions. We show that MgO surface phonon polaritons produce strong near-field enhancements in the central vacuum reaction region of a microcavity. We find that short cavities with thick polar crystal layers yield the largest BIRD enhancements due to enhanced evanescent surface phonon polariton contributions. We further include collisions with a methane bath gas and show that cavity DOS engineering shifts the crossover between BIRD and collisional activation. These results establish Reststrahlen-band DOS engineering as a practical strategy for controlling polyatomic BIRD in infrared microcavities.

physics.chem-ph

Polaritonic control of blackbody infrared radiative dissociation

Vibrational strong light-matter coupling offers a promising approach for controlling chemical reactivity with infrared microcavities. While recent research has examined potential mechanisms for this phenomenon, many important questions remain, including what type of reactions can be modified and to what extent this modification can be achieved. In this study, we explore the dynamics of Blackbody Infrared Radiative Dissociation (BIRD) in microcavities under weak and strong light-matter interaction regimes. Using a Master equation approach, we simulate the effects of infrared field confinement and vibrational strong coupling on BIRD rates for diatomic molecules. We present a framework explaining how infrared microcavities influence BIRD kinetics, highlighting the importance of overtone transitions in the process. Our findings outline the conditions under which significant enhancement or mild suppression of BIRD rates can be achieved, offering insights into the practical limitations and new strategies for controlling chemistry within infrared resonators.

physics.chem-ph

Vibrational polariton transport in disordered media

Chemical reactions and energy transport phenomena have been experimentally reported to be significantly affected by strong light-matter interactions and vibrational polariton formation. These quasiparticles exhibit nontrivial transport phenomena due to the long-range correlations induced by the photonic system and elastic and inelastic scattering processes driven by matter disorder. In this article, we employ the Ioffe-Regel criterion to obtain vibrational polariton mobility edges and to identify distinct regimes of delocalization and transport under variable experimental conditions of light-matter detuning, disorder, and interaction strength. Correlations between the obtained trends and recent observations of polariton effects on reactivity are discussed, and essential differences between transport phenomena in organic electronic exciton and vibrational polaritons are highlighted. Our transport diagrams show the rich diversity of transport phenomena under vibrational strong coupling and indicate that macroscopic delocalization is favored at negative detuning and large light-matter interaction strength. We also find the surprising feature that, despite the presence of dephasing-induced inelastic scattering processes, macroscopic lower polariton delocalization and wave transport are expected to persist experimentally, even in modes with small photonic weight.

physics.chem-ph