Spectral splitting of a stimulated Raman transition in a single molecule

Exploring the interaction of light and matter at the ultimate limit of single photons and single emitters is of great interest both from a fundamental point of view and for emerging applications in quantum engineering. However, the difficulty of generating single photons with specific wavelengths, bandwidths and brightness as well as the weak interaction probability of a single photon with an optical emitter pose a formidable challenge toward this goal. Here, we demonstrate a...

The optical hybridization of the electronic states in strongly coupled molecule-cavity systems have revealed unique properties such as lasing, room temperature polariton condensation, and the modification of excited electronic landscapes involved in molecular isomerization. Here we show that molecular vibrational modes of the electronic ground state can also be coherently coupled with a micro-cavity mode at room temperature, given the low vibrational thermal occupation factor...

Single organic molecules embedded in solid-state matrices exhibit remarkable optical properties, making them competitive candidates for single-photon sources and quantum nonlinear optical elements. However, the lack of long-lived internal states imposes significant constraints on their application in the broader field of quantum technologies. In this article, we reexamine the single-molecule host-guest system from first principles, elaborate on the rich internal states this s...

We propose a method for increasing the Raman scattering from an ensemble of molecules by up to four orders of magnitude. Our method requires an additional coherent source of IR radiation with the half-frequency of the Stokes shift. This radiation excites the molecule electronic subsystem that in turn, via Fr\"ohlich coupling, parametrically excites nuclear oscillations at a resonant frequency. This motion is coherent and leads to a boost of the Raman signal in comparison to t...

When the collective coupling of the rovibrational states in organic molecules and confined electromagnetic modes is sufficiently strong, the system enters into vibrational strong coupling, leading to the formation of hybrid light-matter quasiparticles. In this work we demonstrate theoretically how this hybridization in combination with stimulated Raman scattering can be utilized to widen the capabilities of Raman laser devices. We explore the conditions under which the lasing...

Cavity optomechanics aims to establish optical control over vibrations of mechanical systems, to heat, cool or to drive them toward coherent, or nonclassical states. This field was recently extended to include molecular optomechanics, which describes the dynamics of THz molecular vibrations coupled to the optical fields of lossy cavities via Raman transitions, and was developed to understand the anomalous amplification of optical phonons in Surface-Enhanced Raman Scattering e...

Photophysical and photochemical processes are ruled by the interplay between transient vibrational and electronic degrees of freedom, which are ultimately determined by the multidimensional potential energy surfaces (PESs). Differences between ground and excited PESs are encoded in the relative intensities of resonant Raman bands, but they are experimentally challenging to access requiring measurements at multiple wavelengths under identical conditions. Here we perform a two-...

A single quantum of excitation of a mechanical oscillator is a textbook example of the principles of quantum physics. Mechanical oscillators, despite their pervasive presence in nature and modern technology, do not generically exist in an excited Fock state. In the past few years, careful isolation of GHz-frequency nano-scale oscillators has allowed experimenters to prepare such states at milli-Kelvin temperatures. These developments illustrate the tension between the basic p...

Organic molecules have recently gained attention as novel sources of single photons. We present a joint experiment--theory analysis of the temperature-dependent emission spectra, zero-phonon linewidth, and second-order correlation function of light emitted from a single molecule. We observe spectra with a zero-phonon-line together with several additional sharp peaks, broad phonon sidebands, and a strongly temperature dependent homogeneous broadening. Our model includes both l...

We report coherent association of atoms into a single weakly bound NaCs molecule in an optical tweezer through an optical Raman transition. The Raman technique uses a deeply bound electronic excited intermediate state to achieve a large transition dipole moment while reducing photon scattering. Starting from two atoms in their relative motional ground state, we achieve an optical transfer efficiency of 69%. The molecules have a binding energy of 770.2MHz at 8.83(2)G. This tec...