Single-photon spectroscopy of a single molecule

We employ heterodyne interferometry to investigate the effect of a single organic molecule on the phase of a propagating laser beam. We report on the first phase-contrast images of individual molecules and demonstrate a single-molecule electro-optical phase switch by applying a voltage to the microelectrodes embedded in the sample. Our results may find applications in single-molecule holography, fast optical coherent signal processing, and single-emitter quantum operations.

Quantum mechanical phenomena, such as electronic coherence and entanglement, play a key role in achieving the unrivalled efficiencies of light-energy conversion in natural photosynthetic light-harvesting complexes, and triggered the growing interest in the possibility of organic quantum computing. Since biological systems are intrinsically heterogeneous, clear relations between structural and quantum-mechanical properties can only be obtained by investigating individual assem...

Temporal-spectral modes of light provide a fundamental window into the nature of atomic and molecular systems and offer robust means for information encoding. Methods to precisely characterize the temporal-spectral state of light at the single-photon level thus play a central role in understanding quantum emitters and are a key requirement for quantum technologies that harness single-photon states. Here we demonstrate an optical reference-free method, which melds techniques f...

We point out that individual organic dye molecules, deposited close to optical waveguides on a photonic chip, can act as single photon sources and can also provide localised, giant optical nonlinearities. This new atom-photon interface may be used as a resource for processing quantum information.

Organic dye molecules have been used in great many scientific and technological applications, but their wider use in quantum optics has been hampered by transitions to short-lived vibrational levels, which limit their coherence properties. To remedy this, one can take advantage of optical resonators. Here we present the first results on coherent molecule-resonator coupling, where a single polycyclic aromatic hydrocarbon molecule extinguishes 38\% of the light entering a micro...

Single photons of subnatural linewidth and high spectral brightness are necessary for efficient light-matter interaction at the single photon level, which lies at the heart of many quantum photonic technologies. Here we demonstrate a bright source of single photons with subnatural linewidth, controllable waveforms, and a high spectral brightness of $3.67 \times 10^5$ s$^{-1}$mW$^{-1}$MHz$^{-1}$. The interaction between the single photons and atoms is demonstrated by the contr...

The small cross section of Raman scattering poses a great challenge for its direct study at the single-molecule level. By exploiting the high Franck-Condon factor of a common-mode resonance, choosing a large vibrational frequency difference in electronic ground and excited states and operation at T < 2K, we succeed at driving a coherent stimulated Raman transition in individual molecules. We observe and model a spectral splitting that serves as a characteristic signature of t...

We report on the excitation of single molecules via narrow zero-phonon transitions using short laser pulses. By monitoring the Stokes-shifted fluorescence, we studied the excited state population as a function of the delay time, laser intensity, and frequency detuning. A pi-pulse excitation was demonstrated with merely 500 photons, and 5 Rabi cycles were achieved at higher excitation powers. Our findings are in good agreement with theoretical calculations and provide a first ...

The control and manipulation of quantum-entangled non-local states is a crucial step for the development of quantum information processing. A promising route to achieve such states on a wide scale is to couple solid-state quantum emitters through their coherent dipole-dipole interactions. Entanglement in itself is challenging, as it requires both nanometric distances between emitters and nearly degenerate electronic transitions. Implementing hyperspectral imaging to identify ...

Single molecules in solid-state matrices have been proposed as sources of single-photon Fock states back 20 years ago. Their success in quantum optics and in many other research fields stems from the simple recipes used in the preparation of samples, with hundreds of nominally identical and isolated molecules. Main challenges as of today for their application in photonic quantum technologies are the optimization of light extraction and the on-demand emission of indistinguisha...