Revealing Hidden Vibration Polariton Interactions by 2D IR Spectroscopy

We report the first experimental two-dimensional infrared (2D IR) spectra of novel molecular photonic excitations - vibrational-polaritons. The application of advanced 2D IR spectroscopy onto novel vibrational-polariton challenges and advances our understanding in both fields. From spectroscopy aspect, 2D IR spectra of polaritons differ drastically from free uncoupled molecules; from vibrational-polariton aspects, 2D IR uniquely resolves hybrid light-matter polariton excitations and unexpected dark states in a state-selective manner and revealed hidden interactions between them. Moreover, 2D IR signals highlight the role of vibrational anharmonicities in generating non-linear signals. To further advance our knowledge on 2D IR of vibrational polaritons, we develop a new quantum-mechanical model incorporating the effects of both nuclear and electrical anharmonicities on vibrational-polaritons and their 2D IR signals. This work reveals polariton physics that is difficult or impossible to probe with traditional linear spectroscopy and lays the foundation for investigating new non-linear optics and chemistry of molecular vibrational-polaritons

Spatially Adiabatic Frequency Conversion in Optoelectromechanical Arrays

Faithful conversion of quantum signals between microwave and optical frequency domains is crucial for building quantum networks based on superconducting circuits. Optoelectromechanical systems, in which microwave and optical cavity modes are coupled to a common mechanical oscillator, are a promising route towards this goal. In these systems, efficient, low-noise conversion is possible using a mechanically dark mode of the fields but the conversion bandwidth is limited to a fraction of the cavity linewidth. Here, we show that an array of optoelectromechanical transducers can overcome this limitation and reach a bandwidth that is larger than the cavity linewidth. The coupling rates are varied in space throughout the array so that the mechanically dark mode of the propagating fields adiabatically changes from microwave to optical or vice versa. This strategy also leads to significantly reduced thermal noise with the collective optomechanical cooperativity being the relevant figure of merit. Finally, we demonstrate that, quite surprisingly, the bandwidth enhancement per transducer element is largest for small arrays; this feature makes our scheme particularly attractive for state-of-the-art experimental setups.Comment: 18 pages, 10 figures (including Supplemental Material

Adiabatic State Conversion and Pulse Transmission in Optomechanical Systems

Optomechanical systems with strong coupling can be a powerful medium for quantum state engineering. Here, we show that quantum state conversion between cavity modes with different wavelengths can be realized with high fidelity by adiabatically varying the effective optomechanical couplings. The fidelity for the conversion of gaussian states is derived by solving the Langevin equation in the adiabatic limit. We also show that photon pulses can be transmitted between input-output channels with different wavelengths via the effective optomechanical couplings and the output pulse shape can also be manipulated.Comment: 5 pages, 2 figures. Supplementary Materials at http://prl.aps.org/supplemental/PRL/v108/i15/e15360

Raman Adiabatic Transfer of Optical States

We analyze electromagnetically induced transparency and light storage in an ensemble of atoms with multiple excited levels (multi-Lambda configuration) which are coupled to one of the ground states by quantized signal fields and to the other one via classical control fields. We present a basis transformation of atomic and optical states which reduces the analysis of the system to that of EIT in a regular 3-level configuration. We demonstrate the existence of dark state polaritons and propose a protocol to transfer quantum information from one optical mode to another by an adiabatic control of the control fields