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In this theoretical study, we show how photoelectron signals generated by time-energy entangled photon pairs can monitor ultrafast excited state dynamics of molecules with high joint spectral and temporal resolutions, not limited by the Fourier uncertainty of classical light. This technique scales linearly, rather than quadratically, with the pump intensity, allowing the study of fragile biological samples with low photon fluxes. Since the spectral resolution is achieved by electron detection and the temporal resolution by a variable phase delay, this technique does not require scanning the pump frequency and the entanglement times, which significantly simplifies the experimental setup, making it feasible with current instrumentation. Application is made to the photodissociation dynamics of pyrrole calculated by exact nonadiabatic wave packet simulations in a reduced two nuclear coordinate space. This study demonstrates the unique advantages of ultrafast quantum light spectroscopy.

 

By placing Mg-porphyrin molecules in a chiral optical cavity, time reversal symmetry is broken, and polariton ring currents can be generated with linearly polarized light, resulting in a circular dichroism signal. Since the electronic state degeneracy in the molecule is lifted by the formation of chiral polaritons, this signal is one order of magnitude stronger than the bare molecule signal induced by circularly polarized light. Enantiomer-selective photochemical processes in chiral optical cavities is an intriguing future possibility.