Absorption and fluorescence from single molecules can be tuned by applying an external electric field – a phenomenon known as the Stark effect. A linear Stark effect is associated to a lack of centrosymmetry of the guest in the host matrix. Centrosymmetric guests can display a linear Stark effect in disordered matrices, but the response of individual guest molecules is often relatively weak and non‐uniform, with a broad distribution of the Stark coefficients. Here we introduce a novel single‐molecule host‐guest system, dibenzoterrylene (DBT) in 2,3‐dibromonaphthalene (DBN) crystal. Fluorescent DBT molecules show excellent spectral stability with a large linear Stark effect, of the order of 1.5 GHz/kVcm −1 , corresponding to an electric dipole moment change of around 2 D. Remarkably, when the electric field is aligned with the a crystal axis, nearly all DBT molecules show either positive or negative Stark shifts with similar absolute values. These results are consistent with quantum chemistry calculations. Those indicate that DBT substitutes three DBN molecules along the a ‐axis, giving rise to eight equivalent embedding sites, related by the three glide planes of the orthorhombic crystal. The static dipole moment of DBT molecules is created by host‐induced breaking of the inversion symmetry. This new host–guest system is promising for applications that require a high sensitivity of fluorescent emitters to electric fields, for example to probe weak electric fields.
The local interaction of charges and light in organic solids is the basis of distinct and fundamental effects. We here observe, at the single-molecule scale, how a focused laser beam can locally shift by hundreds of times their natural line width and, in a persistent way, the transition frequency of organic chromophores cooled at liquid helium temperature in different host matrices. Supported by quantum chemistry calculations, the results can be interpreted as effects of a photoionization cascade, leading to a stable electric field, which Stark-shifts the molecular electronic levels. The experimental observation is then applied to a common challenge in quantum photonics, i.e., the independent tuning and synchronization of close-by quantum emitters, which is desirable for multiphoton experiments. Five molecules that are spatially separated by about 50 μm and originally 20 GHz apart are brought into resonance within twice their line width. This tuning method, which does not require additional fabrication steps, is here independently applied to multiple emitters, with an emission line width that is only limited by the spontaneous decay and an inhomogeneous broadening limited to 1 nm. The system hence shows promise for photonic quantum technologies.
Here we introduce a phase-shifting digital holography-based method to determine the temperature profile around an irradiated (sub-)micron spherical bead. The method utilizes a Mach-Zehnder interferometer implemented into an open setup microscope. The results of irradiated gold spheres with diameter of 400 nm and also silver-coated micron-sized silica beads embedded in silicone oil are presented. We show that the applied method is able to accurately determine the surface temperature with accuracy of 1 °C. Our experimental results perfectly confirm the theoretical prediction of temperature profile around the irradiated bead.
The Cover Feature illustrates the spectral tuning of single dibenzoterrylene fluorescent emitters by an external electric field. The matrix‐induced distortion of fluorescent molecules leads to large linear Stark effect. Remarkably, all fluorescent guest molecules show stable and narrow optical transitions with a uniform magnitude of the field response, with two opposite signs. More information can be found in the Article by A. Moradi et al on page 55 in Issue 1, 2019 (DOI: 10.1002/cphc.201800937).
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