Electronic energy relaxation and transition frequency jumps of single molecules at 30 mK

Transition frequency jumps for single terrylene molecules in a polyethylene matrix caused by resonant laser irradiation are investigated at 30 mK. These jumps are not accompanied by substantial sample heating. A model for the effect is: proposed, based on the interaction of tunneling two-level systems (TLSs) surrounding the single molecule with high-energy nonthermal phonons emitted by the molecule during electronic energy relaxation. The radius of the effective interaction volume is estimated to be r(m) approximate to 12.5 nm, and the interaction cross section for nonequilibrium phonon -TLS scattering is estimated as similar to 10(-22) cm(-2)

Light induced single molecule frequency shift

Alight induced frequency shift of the 0-0 line was measured in two-photon excitation spectra of single diphenyloctatetraene molecules doped in a crystal matrix. The shifts were proportional to the laser power with a slope of about 600 MHz/W when the laser beam of about 300 mW power was focused to a diameter of 2 mu m. Significantly, the observed line broadenings were an order of magnitude smaller than the shifts. The effect is ascribed mainly to a ''fast'' energy exchange between a local vibration and thermal phonons created by the third harmonic C-H band absorption in the matrix, and partially to an ac Stark shift

Non-Lorentzian single-molecule line shape: Pseudolocal phonons and coherence transfer

The excitation line shape of a single terrylene molecule in a naphthalene crystal has been investigated. In addition to the conventional Lorentzian, it consists of a dispersive component in the core region and a sideband. This is due to a pseudolocal phonon caused by the substitution of a host molecule with the chromophore. When the pseudolocal phonon is excited, the resonance frequency of the chromophore slightly changes, resulting in the appearance of a second, quasiresonant transition. Coherence transfer between these two optical transitions causes the deviation from the purely Lorentzian line shape

Efficient coupling of photons to a single molecule and the observation of its resonance fluorescence

Single dye molecules at cryogenic temperatures display many spectroscopic phenomena known from free atoms and are thus promising candidates for fundamental quantum optical studies. However, the existing techniques for the detection of single molecules have either sacrificed the information on the coherence of the excited state or have been inefficient. Here we show that these problems can be addressed by focusing the excitation light near to the absorption cross section of a molecule. Our detection scheme allows us to explore resonance fluorescence over 9 orders of magnitude of excitation intensity and to separate its coherent and incoherent parts. In the strong excitation regime, we demonstrate the first observation of the Mollow triplet from a single solid-state emitter. Under weak excitation we report the detection of a single molecule with an incident power as faint as 150 attoWatt, paving the way for studying nonlinear effects with only a few photons.Comment: 6 figure

Ultrafast electronic read-out of diamond NV centers coupled to graphene

Nonradiative transfer processes are often regarded as loss channels for an optical emitter1, since they are inherently difficult to be experimentally accessed. Recently, it has been shown that emitters, such as fluorophores and nitrogen vacancy centers in diamond, can exhibit a strong nonradiative energy transfer to graphene. So far, the energy of the transferred electronic excitations has been considered to be lost within the electron bath of the graphene. Here, we demonstrate that the trans-ferred excitations can be read-out by detecting corresponding currents with picosecond time resolution. We electrically detect the spin of nitrogen vacancy centers in diamond electronically and con-trol the nonradiative transfer to graphene by electron spin resonance. Our results open the avenue for incorporating nitrogen vacancy centers as spin qubits into ultrafast electronic circuits and for harvesting non-radiative transfer processes electronically

Optical microscopy in the nano-world

Scanning near-field optical microscopy (SNOM) is an optical microscopy whose resolution is not bound to the diffraction limit. It provides chemical information based upon spectral, polarization and/or fluorescence contrast images. Details as small as 20 nm can be recognized. Photophysical and photochemical effects can be studied with SNOM on a similar scale. This article reviews a good deal of the experimental and theoretical work on SNOM in Switzerland