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Jochen Feldmann

Publications and source records attributed to Jochen Feldmann.

9 recordsLinked to original sources

Electrical control of Förster energy transfer.

Bringing together compounds of intrinsically different functionality, such as inorganic nanostructures and organic molecules, constitutes a particularly powerful route to creating novel functional devices with synergetic properties found in neither of the constituents. We introduce nanophotonic functional elements combining two classes of materials, semiconductor nanocrystals and dyes, whose physical nature arises as a superposition of the properties of the individual components. The strongly absorbing rod-like nanocrystals focus the incident radiation by photopumping the weakly absorbing dye via energy transfer. The CdSe/CdS nanorods exhibit a large quantum-confined Stark effect on the single-particle level, which enables direct control of the spectral resonance between donor and acceptor required for nanoscopic Förster-type energy transfer in single nanorod-dye couples. With this far-field manipulation of a near-field phenomenon, the emission from single dye molecules can be controlled electrically. We propose that this effect could lead to the design of single-molecule optoelectronic switches providing building blocks for more complex nanophotonic circuitry.

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Efficient intramolecular energy transfer in single endcapped conjugated polymer molecules in the absence of appreciable spectral overlap.

Intramolecular energy transfer is investigated in an endcapped conjugated polymer on the single molecule level at low temperature. While light harvesting in one dimension is on average inefficient in the ensemble, the efficiency scatters widely on the single molecule level, with some molecules exhibiting near-unity transfer probability from the polymer backbone donor to the acceptor endcap. This transfer occurs in the absence of spectral overlap between donor and acceptor, as the electronic and vibronic transitions narrow substantially at low temperatures once inhomogeneous disorder broadening is overcome. The results illustrate how far-field absorption and emission characteristics of molecular transitions are insufficient to describe resonant energy transfer processes following Förster theory in multichromophoric aggregates. Rather, exciton trapping due to efficient multiphonon emission has to be invoked with a possible contribution of strong polaronic coupling.

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How single conjugated polymer molecules respond to electric fields.

Conjugated polymers find applications in a range of devices such as light-emitting diodes, field-effect transistors and solar cells. The elementary electronic response of these semiconductors to electric fields is understood in terms of nanoscale perturbations of charge density. We demonstrate a general breaking of spatial charge symmetry by considering the linear Stark effect in the emission of single chromophores on individual chains. Spectral shifts of several nanometres occur due to effective dipoles exceeding 10 D. Although the electric field does not ionize the exciton, some molecules exhibit field-induced intensity modulations. This quenching illustrates the equivalence of charge symmetry breaking and polaron-pair or charge-transfer-state formation, and provides a microscopic picture of permanent charging, which leads to doping and exciton dissociation in actual devices. In addition to using this tuneable emission in single-photon electro-optic modulators, hysteresis in the Stark shift suggests a route to designing nanoscale memory elements such as molecular switches.

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Semiconductor nanocrystals photosensitize C60 crystals.

Semiconductor nanocrystals (SCNCs) made of CdSe, CdTe, and InP are used to photosensitize needlelike C(60) crystals. The photocurrent is increased by up to 3 orders of magnitude as compared with C(60) crystals without SCNCs. The photocurrent spectrum can be tuned precisely by the SCNC size and material, rendering the SCNC-functionalized C(60) crystals an excellent material for spectrally tuneable photodetectors. We explain the increased photocurrent as a result of photoexcited electrons transferring from the SCNCs to the C(60) crystals and causing photoconductivity, while the complementary holes remain trapped in the SCNCs.

Cadmium Compounds↗

Interplay between Auger and ionization processes in nanocrystal quantum dots.

We study the interplay between Auger effects and ionization processes in the limit of strong electronic confinement in core/shell CdSe/ZnS semiconductor nanocrystal quantum dots. Spectrally resolved fluorescence decay measurements reveal a monotonic increase of the photoluminescence decay rate on excitation density. Our results suggest that Auger recombination accelerates ionization processes that lead to the occupation of dark, nonemissive nanocrystal states. A model is proposed in the quantized Auger regime describing these experimental observations and providing an estimate of the Auger assisted ionization rates.

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A universal picture of chromophores in pi-conjugated polymers derived from single-molecule spectroscopy.

Single-molecule spectroscopy can provide insight into the fundamental photophysics of large macromolecules containing tens of thousands of carbon atoms by circumventing disorder broadening. We apply this technique to comparatively ordered ladder-type poly(para-phenylene) and highly disordered poly(phenylenevinylene) (PPV), both of which are materials of substantial technological interest. Identical spectroscopic features are observed on the single-chromophore level, independent of the chemical structure or the chain morphology. Both materials exhibit narrow fluorescence lines down to 0.5 nm wide, which we attribute to the single-chromophore zero-phonon line, accompanied by a discrete vibronic progression providing a signature of the chemical structure. The chromophore units display spectral diffusion, giving rise to dynamic disorder on the scale of the linewidth. Although the energetic range of spectral diffusion is small, it can influence intramolecular excitation energy transfer and thus the overall molecular emission. The spectral diffusion dynamics of single chromophores are identical in both material systems and follow a universal Gaussian distribution. In the case of emission from multiple chromophores situated on the molecule, which we observe for PPV, spectral diffusion follows Lorentzian-like statistics. The fundamental difference between the two materials is the possibility of coherent interchromophoric coupling in PPV, resulting in strong spectral broadening caused by aggregation or superradiance. Such behavior is absent in the ladder-type polymers, where the linewidth of the emissive species is identical for all molecules. Our results demonstrate that structure-property correlations in conjugated polymers derive mainly from chain morphology rather than chromophoric properties and should be considered extrinsic in nature.

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