Manipulating optical nonlinearities of molecular polaritons by delocalization
Autor: | Joel Yuen-Zhou, Raphael F. Ribeiro, Bo Xiang, Yingmin Li, Wei Xiong, Adam D. Dunkelberger, Blake B. Simpkins |
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Rok vydání: | 2019 |
Předmět: |
Materials science
Photon Population FOS: Physical sciences Physics::Optics 02 engineering and technology 010402 general chemistry 01 natural sciences Condensed Matter::Disordered Systems and Neural Networks Delocalized electron Quantum gate Polariton education Research Articles Condensed Matter::Quantum Gases Condensed Matter - Materials Science education.field_of_study Multidisciplinary business.industry Condensed Matter::Other SciAdv r-articles Materials Science (cond-mat.mtrl-sci) Optics 021001 nanoscience & nanotechnology Polarization (waves) cond-mat.mtrl-sci 0104 chemical sciences Nonlinear system Chemistry Optoelectronics Physics::Accelerator Physics physics.optics Photonics 0210 nano-technology business Physics - Optics Research Article Optics (physics.optics) |
Zdroj: | Science advances, vol 5, iss 9 Science Advances |
Popis: | The macroscopic control of optical nonlinearity is achieved in a cavity polariton due to its delocalized nature. Optical nonlinearities are key resources in the contemporary photonics toolbox, relevant to quantum gate operations and all-optical switches. Chemical modification is often used to control the nonlinear response of materials at the microscopic level, but on-the-fly manipulation of such response is challenging. Tunability of optical nonlinearities in the mid-infrared (IR) is even less developed, hindering its applications in chemical sensing or IR photonic circuitry. Here, we report control of vibrational polariton coherent nonlinearities by manipulation of macroscopic parameters such as cavity longitudinal length or molecular concentration. Further two-dimensional IR investigations reveal that nonlinear dephasing provides the dominant source of the observed ultrafast polariton nonlinearities. The reported phenomena originate from the nonlinear macroscopic polarization stemming from strong coupling between microscopic molecular excitations and a macroscopic photonic cavity mode. |
Databáze: | OpenAIRE |
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