Organic molecule fluorescence as an experimental test-bed for quantum jumps in thermodynamics

Single photon sources (SPSs) based on quantum emitters hold promise in quantum radiometry as metrology standard for photon fluxes at the low light level. Ideally this requires control over the photon flux in a wide dynamic range, sub-Poissonian photon statistics and narrow-band emission spectrum. In this work, a monochromatic single-photon source based on an organic dye molecule is presented, whose photon flux is traceably measured to be adjustable between 144 000 and 1320 00...

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 ...

Electronic conduction through single molecules is affected by the molecular electronic structure as well as by other information that is extremely difficult to assess, such as bonding geometry and chemical environment. The lack of an independent diagnostic technique has long hampered single-molecule conductance studies. We report simultaneous measurement of the conductance and the Raman spectra of nanoscale junctions used for single-molecule electronic experiments. Blinking a...

A main goal of single-molecule experiments is to evaluate equilibrium free energy differences by applying fluctuation relations to repeated work measurements along irreversible processes. We quantify the error that is made in a free energy estimate by means of the Jarzynski equality when the accumulated work expended on the whole system (including the instrument) is erroneously replaced by the work transferred to the subsystem consisting of the sole molecular construct. We fi...

Vibrational levels of the electronic ground states in dye molecules have not been previously explored at high resolution in solid matrices. We present new spectroscopic measurements on single polycyclic aromatic molecules of dibenzoterrylene embedded in an organic crystal made of para-dichlorobenzene. To do this, we use narrow-band continuous-wave lasers and combine spectroscopy methods based on fluorescence excitation and stimulated emission depletion (STED) to assess indivi...

Motivated by recent experiments [Lee et al. Nature 498, 209 (2013)], we present here a detailed theoretical analysis of the Joule heating in current-carrying single-molecule junctions. By combining the Landauer approach for quantum transport with ab initio calculations, we show how the heating in the electrodes of a molecular junction is determined by its electronic structure. In particular, we show that in general the heat is not equally dissipated in both electrodes of the ...

By using the zero-phonon line emission of an individual organic molecule, we realized a source of indistinguishable single photons in the near infrared. A Hong-Ou-Mandel interference experiment is performed and a two-photon coalescence probability of higher than 50% at 2 K is obtained. The contribution of the temperature-dependent dephasing processes to the two-photon interference contrast is studied. We show that the molecule delivers nearly ideal indistinguishable single ph...

Tip-enhanced photoluminescence (TEPL) measurements are performed with sub-nanometer spatial resolution on individual molecules decoupled from a metallic substrate by a thin NaCl layer. TEPL spectra reveal progressive fluorescence quenching with decreasing tip-molecule distance when electrons tunneling from the tip of a scanning tunneling microscope are injected at resonance with the molecular states. Rate equations based on a many-body model reveal that the luminescence quenc...

This paper reviews the recent results in high-resolution spectroscopy on cold molecules. Laser spectroscopy of cold molecules addresses issues of symmetry violation, like in the search for the electric dipole moment of the electron and the studies on energy differences in enantiomers of chiral species; tries to improve the precision to which fundamental physical constants are known and tests for their possible variation in time and space; tests quantum electrodynamics, and se...

We present a simple method to measure the radiative and non-radiative recombination rates of individual fluorescent emitters at room temperature. By placing a single molecule successively close and far from a dielectric interface and simultaneously measuring its photoluminescence decay and its orientation, both the radiative and non-radiative recombination rates can be determined. For CdSe nanocrystals, our results demonstrate that the fluorescence quantum efficiency, determi...