J. Feldmann

Ludwig-Maximilian-University of Munich, München, Bavaria, Germany

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Publications (347)1458.83 Total impact

  • Miao Li, Theobald Lohmüller, Jochen Feldmann
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    ABSTRACT: The controlled injection of nanoscopic objects into living cells with light offers promising prospects for the development of novel molecular delivery strategies or intracellular biosensor applications. Here, we show that single gold nanoparticles from solution can be patterned on the surface of living cells with a continuous wave laser beam. In a second step, we demonstrate how the same particles can then be injected into the cells through a combination of plasmonic heating and optical force. We find that short exposure times are sufficient to perforate the cell membrane and inject the particles into cells with a survival rate of >70%.
    Nano letters. 12/2014;
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    ABSTRACT: We demonstrate strong coupling of nanocavities in metal films, sparked by propagating surface plasmons. Unlike the coupling of metallic nanoparticles which decays over distances of tens of nanometers, the metallic nanocavities display long range coupling at distances of hundreds of nanometers for the properly selected metal/wavelength combinations. Such strong coupling drastically changes the symmetry of the charge distribution around the nanocavities as is evidenced by the nonlinear optical response of the medium. We show that when strongly coupled, equilateral triangular nanocavities lose their individual symmetry to adopt the lower symmetry of the coupled system and respond like a single dipolar entity. A quantitative model is suggested for the transition from individual to strongly coupled nanocavities.
    Journal of optics 11/2014; 16(11):114012. · 2.01 Impact Factor
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    ABSTRACT: Photocatalytic conversion of solar energy to fuels, such as hydrogen, is attracting enormous interest, driven by the promise of addressing both energy supply and storage. Colloidal semiconductor nanocrystals have been at the forefront of these efforts owing to their favourable and tunable optical and electronic properties as well as advances in their synthesis. The efficiency of the photocatalysts is often limited by the slow transfer and subsequent reactions of the photoexcited holes and the ensuing high charge recombination rates. Here we propose that employing a hydroxyl anion/radical redox couple to efficiently relay the hole from the semiconductor to the scavenger leads to a marked increase in the H2 generation rate without using expensive noble metal co-catalysts. The apparent quantum yield and the formation rate under 447 nm laser illumination exceeded 53% and 63 mmol g(-1) h(-1), respectively. The fast hole transfer confers long-term photostability on the system and opens new pathways to improve the oxidation side of full water splitting.
    Nature materials. 08/2014;
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    ABSTRACT: Inspired by biological microswimmer strategies, we consider the design of helical silica particles. We characterize optically induced rotation of these “microscrews”, and discuss their applications as highly controlled microswimmers in the low Reynold’s number regime.
    CLEO: Science and Innovations; 06/2014
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    ABSTRACT: We report on a combined study of Rayleigh and Raman scattering spectroscopy, 3D electron tomography, and discrete dipole approximation (DDA) calculations of a single complex shaped gold nanoparticle (NP). Using the exact reconstructed 3D morphology of the NP as input for the DDA calculations, the experimental results can be reproduced with unprecedented precision and detail. We find that not only the exact NP morphology but also the surroundings including the points of contact with the substrate are of crucial importance for a correct prediction of the NP optical properties. The achieved accuracy of the calculations allows determining how many of the adsorbed molecules have a major contribution to the Raman signal, a fact that has important implications for analyzing experiments and designing sensing applications.
    ACS Nano 04/2014; · 12.03 Impact Factor
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    ABSTRACT: We report that plasmonic nanoantennas made by DNA origami can be used as reliable and efficient probes for surface enhanced Raman spectroscopy (SERS). The nanoantenna is built up by two gold nanoparticles that are linked together by a three-layered DNA origami block at a separation distance of 6 nm in order to achieve plasmonic coupling and the formation of a plasmonic 'hot spot'. The plasmonic properties of the hybrid structure are optically characterized by dark-field imaging and polarization-dependent spectroscopy. SERS measurements on molecules that are embedded in the DNA origami which bridges the nanoantenna gap were performed in order to demonstrate the excellent performance of these structures for enhancing spectroscopic signals. A strong enhancement of the Raman signal was recorded from measurements on single hot spots compared to measurements in bulk. Finally, we show that the laser polarization with respect to the dimer orientation has a strong impact on the SERS performance.
    Nano Letters 04/2014; · 13.03 Impact Factor
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    ABSTRACT: Selected Lectures Presented at Symposium on Ultrafast Dynamics of the 7th International Conference on Materials for Advanced TechnologiesSingapore, 30 June – 5 July 2013Edited by: G G Gurzadyan (NTU, Singapore), G Lanzani (Istituto Italiano di Tecnologia, Italy), C Soci (NTU, Singapore), T C Sum (NTU, Singapore)
    Selected Lectures Presented at Symposium on Ultrafast Dynamics of the 7th International Conference on Materials for Advanced Technologies; 04/2014
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    ABSTRACT: Rod-shaped CdTe–Cu2−xTe nano-heterostructures with tunable dimensions of both sub-units and a type II band alignment were prepared by Cd2+/Cu+ cation exchange. The light absorption properties of the heterostructures are dominated by the excitonic and plasmonic contributions arising, respectively, from the CdTe and the Cu2−xTe sub-units. These results were confirmed over a wide range of sub-unit length fractions through optical modelling based on the discrete dipole approximation (DDA). Although assuming electronically independent sub-units, our modelling results indicate a negligible ground state interaction between the CdTe exciton and the Cu2−xTe plasmon. This lack of interaction may be due to the low spectral overlap between exciton and plasmon, but also to localization effects in the vacancy-doped sub-unit. The electronic interaction between both sub-units was evaluated with pump-probe spectroscopy by assessing the relaxation dynamics of the excitonic transition. In particular, the CdTe exciton decays faster in the presence of the Cu2−xTe sub-unit, and the decay gets faster with increasing its length. This points towards an increased probability of Auger mediated recombination due to the high carrier density in the Cu2−xTe sub-unit. This indication is supported through length-fraction dependent band structure calculations, which indicate a significant leakage of the CdTe electron wavefunction into the Cu2−xTe sub-unit that increases along with the shortening of the CdTe sub-unit, thus enhancing the probability of Auger recombination. Therefore, for the application of type II chalcogenide–chalcogenide heterostructures based on Cu and Cd for photoenergy conversion, a shorter Cu-based sub-unit may be advantageous, and the suppression of high carrier density within this sub-unit is of high importance.
    J. Mater. Chem. C. 04/2014; 2(17).
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    ABSTRACT: This feature article discusses the optical trapping and manipulation of plasmonic nanoparticles, an area of current interest with potential applications in nanofabrication, sensing, analytics, biology and medicine. We give an overview over the basic theoretical concepts relating to optical forces, plasmon resonances and plasmonic heating. We discuss fundamental studies of plasmonic particles in optical traps and the temperature profiles around them. We place a particular emphasis on our own work employing optically trapped plasmonic nanoparticles towards nanofabrication, manipulation of biomimetic objects and sensing.
    Nanoscale 03/2014; · 6.73 Impact Factor
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    ABSTRACT: The sensitization of dispersed P25 TiO2 nanoparticles (NPs) and macroporous TiO2 films with water-soluble and air-stable PbS quantum dots (QDs) capped with l-glutathione (GSH) ligands was investigated. Optimum sensitization was achieved by careful adjustment of the surface charges of TiO2 and PbS QDs by controlling the pH of the QD solution. Efficient electron transfer from photoexcited PbS QDs via the GSH ligands into the conduction band of TiO2 was demonstrated by photoluminescence (PL) spectroscopy of PbS-sensitized P25 nanoparticles. The PbS QD-sensitized porous TiO2 electrodes were used to prepare quantum-dot-sensitized solar cells (QDSSCs) utilizing a CuxSy counter electrode and aqueous polysulfide electrolyte. Cells with up to 64% injection efficiency, 1.1% AM 1.5 conversion efficiency, and short circuit current density of 7.4 mA cm–2 were obtained. The physical parameters of the cells were investigated using impedance spectroscopy.
    The Journal of Physical Chemistry C. 03/2014; 118(10):5142–5149.
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    ABSTRACT: When two or more metallic nanoparticles are in close proximity, their plasmonic modes may interact through the near field, leading to additional resonances of the coupled system or to shifts of their resonant frequencies. This process is analogous to atom-hybridization, as had been proposed by Gersten and Nitzan and modeled by Nordlander et al. The coupling between plasmonic modes can be in-phase (symmetric) or out-of-phase (anti-symmetric), reflecting correspondingly, the "bonding" and "anti-bonding" nature of such configurations. Since the incoming light redistributes the charge distribution around the metallic nanoparticles, its polarization features play a major role in the nonlinear optical probing of the energy-level landscape upon hybridization. Thus, controlling the nature of coupling between metallic nanostructures is of a great importance as it enables tuning their spectral responses leading to novel devices which may surpass the diffraction limit.
    02/2014;
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    ABSTRACT: A mesoporous electron-donor covalent organic framework based on a benzodithiophene core, BDT-COF, was obtained through condensation of a benzodithiophene-containing diboronic acid and hexahydroxytriphenylene (HHTP). BDT-COF is a highly porous, crystalline and thermally stable material, which can be handled in air. Highly porous, crystalline oriented thin BDT-COF films were synthesized from solution on different polycrystalline surfaces, indicating the generality of the synthetic strategy. The favorable orientation, crystallinity, porosity and the growth mode of the thin BDT-COF films were studied by means of X-ray diffraction (XRD), 2D grazing incidence diffraction (GID), transmission and scanning electron microscopy (TEM, SEM) and krypton sorption. The highly porous thin BDT-COF films were infiltrated with soluble fullerene derivatives, such as [6,6]-phenyl C61 butyric acid methyl ester (PCBM), to obtain an interpenetrated electron-donor/acceptor host-guest system. Light-induced charge transfer from the BDT-framework to PCBM acceptor molecules was indicated by efficient photoluminescence quenching. Moreover, we monitored the dynamics of photo-generated hole-polarons via transient absorption spectroscopy. This work represents a combined study of the structural and optical properties of highly oriented mesoporous thin COF films serving as host for the generation of periodic interpenetrated electron-donor and electron-acceptor systems.
    ACS Nano 02/2014; · 12.03 Impact Factor
  • Wei Li, Thomas Dittrich, Frank Jäckel, Jochen Feldmann
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    ABSTRACT: Pyrite nanocrystals are currently considered as a promising material for large scale photovoltaic applications due to their non-toxicity and large abundance. While scalable synthetic routes for phase-pure and shape controlled colloidal pyrite nanocrystals have been reported, their use in solar cells has been hampered by the detrimental effects of their surface defects. Here, we report a systematic study of optical and electronic properties of pyrite nanocrystal thin films employing a series of different ligands varying both the anchor and bridging group. The effect of the ligands on the optical and electronic properties is investigated by UV-vis/NIR absorption spectroscopy, current voltage characteristic measurements and surface photovoltage spectroscopy. We find that the optical absorption is mainly determined by the anchor group. The absorption onset in the thin films shifts up to ∼100 meV to the red. This is attributed to changes in the dielectric environment induced by different anchors. The conductivity and photoconductivity, on the other hand, are determined by combined effects of anchor and bridging group, which modify the effective hopping barrier. Employing different ligands, the differential conductance varies over four orders of magnitude. The largest redshift and differential conductance are observed for ammonium sulfides and thiolated aromatic linkers. Pyridine and long chain amines, on the other hand, lead to smaller modifications. Our findings highlight the importance of surface functionalization and interparticle electronic coupling in the use of pyrite nanocrystals for photovoltaic devices.
    Small 01/2014; · 7.82 Impact Factor
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    ABSTRACT: We report on a highly sensitive approach to measure and quantify the time dependent changes of the flow generated by the flagella bundle rotation of single bacterial cells. This is achieved by observing the interactions between a silica particle and a bacterium, which are both trapped next to each other in a dual beam optical tweezer. In this configuration, the particle serves as a sensitive detector where the fast-Fourier analysis of the particle trajectory renders, it possible to access information about changes of bacterial activity.
    Applied Physics Letters 01/2014; 104(9):093701-093701-5. · 3.52 Impact Factor
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    ABSTRACT: We demonstrate how optical tweezers may provide a sensitive tool to analyze the fluidic vibrations generated by the movement of small aquatic organisms. A single gold nanoparticle held by an optical tweezer is used as a sensor to quantify the rhythmic motion of a Nauplius larva (Artemia salina) in a water sample. This is achieved by monitoring the time dependent displacement of the trapped nanoparticle as a consequence of the Nauplius activity. A Fourier analysis of the nanoparticle's position then yields a frequency spectrum that is characteristic to the motion of the observed species. This experiment demonstrates the capability of this method to measure and characterize the activity of small aquatic larvae without the requirement to observe them directly and to gain information about the position of the larvae with respect to the trapped particle. Overall, this approach could give an insight on the vitality of certain species found in an aquatic ecosystem and could expand the range of conventional methods for analyzing water samples.
    Journal of visualized experiments : JoVE. 01/2014;
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    ABSTRACT: The self-assembly of nanoscale elements into three-dimensional structures with precise shapes and sizes is important in fields such as nanophotonics, metamaterials and biotechnology. Short molecular linkers have previously been used to create assemblies of nanoparticles, but the approach is limited to small interparticle distances, typically less than 10 nm. Alternatively, DNA origami can precisely organize nanoscale objects over much larger length scales. Here we show that rigid DNA origami scaffolds can be used to assemble metal nanoparticles, quantum dots and organic dyes into hierarchical nanoclusters that have a planet-satellite-type structure. The nanoclusters have a tunable stoichiometry, defined distances of 5-200 nm between components, and controllable overall sizes of up to 500 nm. We also show that the nanoscale components can be positioned along the radial DNA spacers of the nanostructures, which allows short- and long-range interactions between nanoparticles and dyes to be studied in solution. The approach could, in the future, be used to construct efficient energy funnels, complex plasmonic architectures, and porous, nanoengineered scaffolds for catalysis.
    Nature Nanotechnology 12/2013; · 31.17 Impact Factor
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    ABSTRACT: An optical printing technique is used to accurately position a 150 nm diameter gold nanoparticle onto a submicrometer linear three-hole defect of a photonic crystal nanocavity. It is shown (using both experiment and finite-difference time domain modelling), that there is an electromagnetic interaction between the nanoparticle and the cavity mode, with the electromagnetic field within the cavity being dissipated by driving the nanoparticle plasmon resonance. The use of a printing technique to selectively position nanoparticles onto a surface-accessible cavity potentially allows the hybridisation between electronic, excitonic, and optical states to be explored with high precision. Furthermore, through its scalable nature it also opens possibilities for the routine construction of new types of photonic devices and sensors.
    Advanced Optical Materials. 12/2013; 1(12).
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    ABSTRACT: The photocatalytic water reduction reaction on CdS nanorods was studied as function of Pt cluster size. Maximum H2 production is found for Pt46. This effect is attributed to the size dependent electronic properties (e.g. LUMO) of the clusters with respect to the band edges of the semiconductor. This observation may be applicable for the study and interpretation of other systems and reactions, e.g. H2O oxidation or CO2 reduction.
    Journal of the American Chemical Society 08/2013; · 10.68 Impact Factor
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    ABSTRACT: Noble metal particles feature intriguing optical properties, which can be utilized to manipulate them by means of light. Light absorbed by gold nanoparticles, for example, is very efficiently converted into heat and single particles can thus be used as a fine tool to apply heat to a nanoscopic area. At the same time, gold nanoparticles are subject to optical forces when they are irradiated with a focused laser beam which renders it possible to print, manipulate, and optically trap them in two- and three dimensions. Here, we demonstrate how these properties can be used to control the polymerization reaction and thermal curing of polydimethylsiloxane (PDMS) at the nanoscale and how these findings can be applied to synthesize polymer nanostructures such as particles and nanowires with sub-diffraction limited resolution.
    ACS Nano 08/2013; · 12.03 Impact Factor
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    ABSTRACT: We report on the deposition of individual gold nanorods from an optical trap using two different laser wavelengths. Laser light, not being resonant to the plasmon resonances of the nanorods, is used for stable trapping and in situ alignment of individual nanorods. Laser light, being resonant to the transversal mode of the nanorods, is used for depositing nanorods at desired locations. The power and polarization dependence of the process is investigated and discussed in terms of force balances between gradient and scattering forces, plasmonic heating, and rotational diffusion of the nanorods. This two-color approach enables faster printing than its one-color equivalent and provides control over the angular orientation (±16°) and location of the deposited nanorods at the single-nanorod level.
    Nano Letters 08/2013; · 13.03 Impact Factor

Publication Stats

7k Citations
1,458.83 Total Impact Points

Institutions

  • 1997–2014
    • Ludwig-Maximilian-University of Munich
      • Photonics and Optoelectronics Group
      München, Bavaria, Germany
  • 2011
    • International Institute of Information Technology, Hyderabad
      Bhaganagar, Andhra Pradesh, India
  • 2008
    • University of Chicago
      Chicago, Illinois, United States
  • 2007
    • Technische Universität Dresden
      Dresden, Saxony, Germany
  • 1987–2006
    • Philipps University of Marburg
      • Faculty of Physics
      Marburg, Hesse, Germany
  • 2003
    • Humboldt-Universität zu Berlin
      Berlín, Berlin, Germany
  • 2001
    • University of Colorado at Boulder
      Boulder, Colorado, United States
  • 1999–2001
    • University of Technology Munich
      • Walter Schottky Institut (WSI)
      München, Bavaria, Germany
    • University of Münster
      Muenster, North Rhine-Westphalia, Germany
  • 1993
    • University of Wuerzburg
      • Institute of Physics
      Würzburg, Bavaria, Germany
  • 1992
    • Heriot-Watt University
      • Department of Physics
      Edinburgh, SCT, United Kingdom
  • 1989
    • Phillips University
      Missouri, United States