Abstract
Several years ago, strong coupling between electronic molecular transitions and photonic structures was shown to modify the electronic landscape of the molecules and affect their chemical behavior. Since then, this concept has evolved into a new field known as polaritonic chemistry. An important ingredient in the progress of this field was the demonstration of strong coupling with intra-molecular vibrations, which enabled the modification of processes occurring at the electronic ground-state. Here we demonstrate strong coupling with collective, inter-molecular vibrations occurring in organic materials in the low-terahertz region (lesssim1012 Hz). Using a cavity filled with α-lactose molecules, we measure the temporal evolution and observe coherent Rabi oscillations, corresponding to a splitting of 68 GHz. These results take strong coupling into a new class of materials and processes, including skeletal polymer motions, protein dynamics, metal organic frameworks and other materials, in which collective, spatially extended degrees of freedom participate in the dynamics.
Highlights
Several years ago, strong coupling between electronic molecular transitions and photonic structures was shown to modify the electronic landscape of the molecules and affect their chemical behavior
Strongly coupled organic systems involved the coupling of an optical resonance to electronic transitions in molecules (Frenkel excitons), recently, vibrational strong coupling has been introduced as a new paradigm[31,32,33,34,35,36]
A different class of vibrational modes in organic materials are inter-molecular vibrations, which are relevant in large molecular structures such as organic crystalline materials, polymers, and proteins
Summary
Strong coupling between electronic molecular transitions and photonic structures was shown to modify the electronic landscape of the molecules and affect their chemical behavior. The creation of the polaritonic wavefunctions under strong coupling and the modification of the energetic landscape of the molecules can have a significant influence on the physical and chemical properties of the molecules[1,15,16], affecting the rates and yields of chemical reactions[17,18,19,20,21,22], their emission properties[23,24,25], electronic and excitonic transport[26,27,28,29,30] and more This new field, known as polaritonic chemistry, is currently under intense study, both experimentally and theoretically. A different class of vibrational modes in organic materials are inter-molecular vibrations, which are relevant in large molecular structures such as organic crystalline materials, polymers, and proteins These vibrations, which typically lie in the terahertz frequency regime (1011–1013 Hz, or several tens of cm−1), correspond to the concerted motion of the unit cells, one with respect to another (rather than internal vibrations of atoms within each molecule). Our results extend the applicability of polaritonic chemistry to a plethora of large-scale organic systems, such as biological macromolecules[39], polymer chains[40], energetic materials with low lying collective vibrations[41], skeletal motions in metal organic frameworks (MOFs)[42], and many others
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