Spectral splitting of a stimulated Raman transition in a single molecule

Stimulated Raman scattering (SRS) has played an increasingly pivotal role in chemistry and photonics. Recently, understanding of light-molecule interaction during SRS was brought to a new quantitative level through the introduction of stimulated Raman cross section, $\sigma_{SRS}$. Measurements of Raman-active molecules have revealed interesting insights, and theoretical consideration has suggested an Einstein-coefficient-like relation between $\sigma_{SRS}$ and the commonly ...

We propose a method for achieving highly efficient transfer between the vibrational states in a diatomic molecule. The process is mediated by strong laser pulses and can be understood in terms of light-induced potentials. In addition to describing a specific molecular system, our results show how, in general, one can manipulate the populations of the different quantum states in double well systems.

Direct detection of single photons at wavelengths beyond 2 microns under ambient conditions remains an outstanding technological challenge. One promising approach is frequency upconversion into the visible (VIS) or near-infrared (NIR) domain, where single photon detectors are readily available. Here, we propose a nanoscale solution based on a molecular optomechanical platform to up-convert photons from the far and mid-infrared (covering part of the THz gap) into the VIS-NIR d...

The unusual features of quantum mechanics are enabling the development of technologies not possible with classical physics. These devices utilize nonclassical phenomena in the states of atoms, ions, and solid-state media as the basis for many prototypes. Here we investigate molecular states as a distinct alternative. We demonstrate a memory for light based on storing photons in the vibrations of hydrogen molecules. The THz-bandwidth molecular memory is used to store 100-fs pu...

Preparing molecules at rest and in a highly pure quantum state is a long standing dream in chemistry and physics, so far achieved only for a select set of molecules in dedicated experimental setups. Here, a quantum-limited combination of mass spectrometry and Raman spectroscopy is proposed that should be applicable to a wide range of molecular ions. Excitation of electrons in the molecule followed by uncontrolled decay and branching into several lower energy states is avoided...

From the high vibrational dipolar strength offered by molecular liquids, we demonstrate that a molecular vibration can be ultra-strongly coupled to multiple IR cavity modes, with Rabi splittings reaching $24\%$ of the vibration frequencies. As a proof of the ultra-strong coupling regime, our experimental data unambiguously reveal the contributions to the polaritonic dynamics coming from the anti-resonant terms in the interaction energy and from the dipolar self-energy of the ...

Many physical systems display quantized energy states. In optics, interacting resonant cavities show a transmission spectrum with split eigenfrequencies, similar to the split energy levels that result from interacting states in bonded multi-atomic, i.e. molecular, systems. Here, we study the nonlinear dynamics of photonic diatomic molecules in linearly coupled microresonators and demonstrate that the system supports the formation of self-enforcing solitary waves when a laser ...

In this article, we address the optomechanical effects in surface-enhanced resonant Raman scattering (SERRS) from a single molecule in a nano-particle on mirror (NPoM) nanocavity by developing a quantum master equation theory, which combines macroscopic quantum electrodynamics and electron-vibration interaction within the framework of open quantum system theory. We supplement the theory with electromagnetic simulations and time-dependent density functional theory calculations...

We demonstrate a novel technique of coherent Raman spectroscopy with a femtosecond laser. We apply to a molecular sample a sequence of pairs of ultrashort excitation and probe pulses, with a linearly increasing time delay between the two pulses from one pair to the next. We measure, as a function of the delay, the intensity modulation in the signal resulting from the differential detection of the Stokes and anti-Stokes radiations generated at the sample. The Fourier transform...

We present a general and highly efficient scheme for performing narrow-band Raman transitions between molecular vibrational levels using a coherent train of weak pump-dump pairs of shaped ultrashort pulses. The use of weak pulses permits an analytic description within the framework of coherent control in the perturbative regime, while coherent accumulation of many pulse pairs enables near unity transfer efficiency with a high spectral selectivity, thus forming a powerful comb...