Theory of Novel Quantum Nonlinear Spectroscopy for Molecular Relaxation and Radiative Processes in Nanoscale

Project: Research

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The quantum nature of particles predicted from quantum mechanics has shown many spooky properties. One of the striking features is the photon entanglement which is of particular interest for encrypted communication, computing and material detections. Moreover, the nonclassical bandwidth features of the quantum states of light have long been recognized as a potential resource for quantum-enhanced applications. Extensive studies have demonstrated recently the advantage of improving the sensitivity and signal-to-noise ratio by the entangled photons. While existing research provide some new perspective on the quantum-enhanced detections of material properties, the quantum light is referred to as a “quantum gap” in optical spectroscopy normally having different goals from quantum optics. The spectroscopic study of material properties is inevitably limited by using simple classical light. The limited resolution and sensitivity from classical pulses have becomemajor bottleneckfor the future development of spectroscopic technologies. This project aims to tackle this bottleneck by developing the state-of-the-art quantum-light nonlinear spectroscopy for complex molecules, as the quantum states of light provide novel control knobs such as entanglement time and squeezing for the spectroscopic technique. On one hand, the complete for the nonlinear signals will be developed using Green’s function technique, to incorporate the complex molecular dynamics. We shall further combine the quantum-light signals with nonlinear interferometry, as parts of new detection schemes for better resolution and sensitivity. The key challenge here is the nonlinearity from the many-particle effects and the strong field-matter interactions, demanding the knowledgebeyondthe 3rd order susceptibilities of molecules. To this end, thenon-perturbativeapproaches will be developed in the proposed research, in light of the molecular polaritons resulting from the strong interaction with the fields in microcavities and electromagnetic nanostructure. This project, on the other hand, will substantially explore the relaxation and ultrafast electron dynamics of molecular polaritons, in the presence of inhomogeneous dephasing and nonlinearity upon many-particle excitations. A family of quantum-light nonlinear spectroscopic probes will be developed to capture the real-time dynamics of polaritons, as a key part of understanding the molecular relaxation processes in nanoscale. The successful accomplishment of this project will deliver a proof-of-principle quantum nonlinear spectroscopic technique greatly exceeding the bounds of temporal and spectral resolutions and sensitivity given by the classical spectroscopic paradigm. We expect to unveil new information about the motions of electrons and vibrations in nanomaterials, which will greatly advance the fields of nanophotonics and the quantum imaging of microscopic-scaled objects.  


Project number9048216
Grant typeECS
Effective start/end date1/01/22 → …