We present the concept of electrostatic field-driven supra-molecular translation within electrically connected plasmonic nano-antennas. The antenna serves as an anchoring point for the mechanically interlocked molecules, as an electrode for the electrostatic field, and as an amplifier of the antenna-enhanced fluorescence. The synthesis of a push–pull donor–π–acceptor chromophore with optical properties aligned to the antenna resonance is described and its immobilization on the surface is demonstrated. Photoluminescence experiments of the chromophore on a gold nano-antenna are shown, highlighting the molecule–antenna coupling and resulting emission intensity increase. The successful synthesis of an electrostatic field-sensitive rotaxane in water is described and the tightrope walk between functionality and water solubility is illustrated by unsuccessful designs. In solution, an enhanced fluorescence quantum yield is observed for the chromophore comprising the mechanically interlocked rotaxane in water and DMSO compared to the reference rod, ideal for future experiments in plasmonic nano-antennas.
L. Jucker, M. Ochs, R. Kullock, Y. Aeschi, B. Hecht, M. Mayor
Organic Materials, 4, 127-136 (2022)
The control of nonlinear optical signals in nanostructured systems is pivotal to develop functional devices suitable for integration in optical platforms. A possible control mechanism is exploiting coherent interactions between different nonlinear optical processes. Here, this concept is implemented by taking advantage of the strong field enhancement and high optical non-linearity provided by plasmonic nanostructures. Two beams, one at the angular frequency ω, corresponding to the telecom wavelength λ= 1551 nm, and the other at 2ω, are combined to generate a sum-frequency signal at 3ω from single asymmetric gold nanoantennas. This nonlinear signal interferes with the third-harmonic radiation generated by the beam at ω, resulting in a modulation up to 50% of the total signal at 3ω depending on the relative phase between the beams. Such a large intensity modulation of the nonlinear signal is accompanied by a rotation of its polarization axis, due to the lack of central symmetry of the nanostructure. The demonstration that the nonlinear emission can be coherently controlled through the phase difference of the two-color illumination represents a promising route toward all-optical logic operations at the nanoscale through nonlinear optical signal manipulation.
A. D. Francescantonio, A. Locatelli, X. Wu, A. Zilli, T. Feichtner, P. Biagioni, L. Duò, D. Rocco, C. D. Angelis, M. Celebrano, B. Hecht and M. Finazzi
Adv. Optical Mater, 2200757 (2022)
Visible and infrared photons can be detected with a broadband response via the internal photoeffect. By using plasmonic nanostructures, i.e. nanoantennas, wavelength selectivity can be introduced to such detectors through geometry-dependent resonances. Also, additional functionality, like electronic responsivity switching and polarization detection have been realized. However, previous devices consisted of large arrays of nanostructures to achieve detectable photocurrents. Here we show that this concept can be scaled down to a single antenna level, resulting in detector dimensions well below the resonance wavelength of the device. Our design consists of a single electrically-connected plasmonic nanoantenna covered with a wide-bandgap semiconductor allowing broadband photodetection in the VIS/NIR via injection of hot carriers. We demonstrate electrical switching of the color sensitivity as well as polarization detection. Our results hold promise for the realization of ultra small, highly integratable photodetectors with advanced functionality.
P. Petsch, R. Kullock, V. Gabriel, L. Zurak, M. Emmerling, B. Hecht
When photons interact with matter, forces and torques occur due to the transfer of linear and angular momentum, respectively. The resulting accelerations are small for macroscopic objects but become substantial for microscopic objects with small masses and moments of inertia, rendering photon recoil very attractive to propel micro- and nano-objects. However, until now, using light to control object motion in two or three dimensions in all three or six degrees of freedom has remained an unsolved challenge. Here we demonstrate light-driven microdrones (size roughly 2 μm and mass roughly 2 pg) in an aqueous environment that can be manoeuvred in two dimensions in all three independent degrees of freedom (two translational and one rotational) using two overlapping unfocused light fields of 830 and 980 nm wavelength. To actuate the microdrones independent of their orientation, we use up to four individually addressable chiral plasmonic nanoantennas acting as nanomotors that resonantly scatter the circular polarization components of the driving light into well-defined directions. The microdrones are manoeuvred by only adjusting the optical power for each motor (the power of each circular polarization component of each wavelength). The actuation concept is therefore similar to that of macroscopic multirotor drones. As a result, we demonstrate manual steering of the microdrones along complex paths. Since all degrees of freedom can be addressed independently and directly, feedback control loops may be used to counteract Brownian motion. We posit that the microdrones can find applications in transport and release of cargos, nanomanipulation, and local probing and sensing of nano and mesoscale objects.
Future photonic devices require efficient, multifunctional, electrically driven light sources with directional emission properties and subwavelength dimensions. Electrically driven plasmonic nanoantennas have been demonstrated as enabling technology. Here, we present the concept of a nanoscale organic light-emitting antenna (OLEA) as a color- and directionality-switchable point source. The device consists of laterally arranged electrically contacted gold nanoantennas with their gap filled by the organic semiconductor zinc phthalocyanine (ZnPc). Since ZnPc shows preferred hole conduction in combination with gold, the recombination zone relocates depending on the polarity of the applied voltage and couples selectively to either of the two antennas. Thereby, the emission characteristics of the device also depend on polarity. Contrary to large-area OLEDs where recombination at metal contacts significantly contributes to losses, our ultracompact OLEA structures facilitate efficient radiation into the far-field rendering transparent electrodes obsolete. We envision OLEA structures to serve as wavelength-scale pixels with tunable color and directionality for advanced display applications.
P. Grimm, S. Zeißner, M. Rödel, S. Wiegand, S. Hammer, M. Emmerling, E. Schatz, R. Kullock, J Pflaum, B. Hecht
Nano Lett., 1c03994 (2022)
Coupling N identical emitters to the same field mode is a well-established method to enhance light-matter interaction. However, the resulting √N boost of the coupling strength comes at the cost of a “linearized” (effectively semiclassical) dynamics. Here, we instead demonstrate a new approach for enhancing the coupling constant of a single quantum emitter, while retaining the nonlinear character of the light-matter interaction. We consider a single quantum emitter with N nearly degenerate transitions that are collectively coupled to the same field mode. We show that in such conditions an effective Jaynes-Cummings model emerges with a boosted coupling constant of order √N. The validity and consequences of our general conclusions are analytically demonstrated for the instructive case N=2. We further observe that our system can closely match the spectral line shapes and photon autocorrelation functions typical of Jaynes-Cummings physics, proving that quantum optical nonlinearities are retained. Our findings match up very well with recent broadband plasmonic nanoresonator strong-coupling experiments and will, therefore, facilitate the control and detection of single-photon nonlinearities at ambient conditions.
T. Tufarelli, D. Friedrich, H. Groß, J. Hamm, O. Hess, B. Hecht
Phys. Rev. Research 3, 033103 (2021)
Unlocking the true potential of optical spectroscopy on the nanoscale requires development of stable and low-noise laser sources. Here,we have developed a low-noise supercontinuum (SC) source based on an all-normal dispersion fiber pumped by a femtosecond fiber laserand demonstrate high resolution, spectrally resolved near-field measurements in the near-infrared (NIR) region. Specifically, we explore thereduced-noise requirements for aperture-less scattering-type scanning near-field optical microscopy (s-SNOM), including inherent pulse-to-pulse fluctuation of the SC. We use our SC light source to demonstrate the first NIR, spectrally resolved s-SNOM measurement, a situationwhere state-of-the-art commercial SC sources are too noisy to be useful. We map the propagation of surface plasmon polariton (SPP) waveson monocrystalline gold platelets in the wavelength region of 1.34–1.75μm in a single measurement, thereby characterizing experimentallythe dispersion curve of the SPP in the NIR. Our results represent a technological breakthrough that has the potential to enable a wide rangeof new applications of low-noise SC sources in near-field studies.
K. J. Kaltenecker, Shreesha Rao D. S., M. Rasmussen, H. B. Lassen, E. J. R. Kelleher, E. Krauss, B. Hecht, N. A. Mortensen, L. Grüner-Nielsen, C. Markos, O. Bang, N. Stenger, P. U. Jepsen
APL Photonics 6, 066106 (2021)
The electrical excitation of guided plasmonic modes at the nanoscale enables integration of optical nanocircuitry into nanoelectronics. In this context, exciting plasmons with a distinct modal field profile constitutes a key advantage over conventional single-mode integrated photonics. Here, we demonstrate the selective electrical excitation of the lowest-order symmetric and antisymmetric plasmonic modes in a two-wire transmission line. We achieve mode selectivity by precisely positioning nanoscale excitation sources, i.e., junctions for inelastic electron tunneling, within the respective modal field distribution. By using advanced fabrication that combines focused He-ion beam milling and dielectrophoresis, we control the location of tunnel junctions with sub-10 nm accuracy. At the far end of the two-wire transmission line, the guided plasmonic modes are converted into far-field radiation at separate spatial positions showing two distinct orthogonal polarizations. Hence, the resulting device represents the smallest electrically driven light source with directly switchable polarization states with possible applications in display technology.
M. Ochs, L. Zurak, E. Krauss, J. Meier, M. Emmerling, R. Kullock, B. Hecht
Coherent perfect absorption (CPA) describes the absence of all outgoing modes from a lossy resonator, driven by lossless incoming modes. Here, we show that for nanoresonators that also exhibit radiative losses, e.g., plasmonic nanoantennas, a generalized version of CPA (gCPA) can be applied. In gCPA outgoing modes are suppressed only for a subset of (guided plasmonic) modes while other (radiative) modes are treated as additional loss channels - a situation typically referred to as perfect impedance matching. Here we make use of gCPA to show how to achieve perfect impedance matching between a single nanowire plasmonic waveguide and a plasmonic nanoantenna. Antennas with both radiant and subradiant characteristics are considered. We further demonstrate potential applications in background-free sensing.
Yagi-Uda antennas are a key technology for efficiently transmitting information from point to point using radio waves. Since higher frequencies allow higher bandwidths and smaller footprints, a strong incentive exists to shrink Yagi-Uda antennas down to the optical regime. Here we demonstrate electrically-driven Yagi-Uda antennas for light with wavelength-scale footprints that exhibit large directionalities with forward-to-backward ratios of up to 9.1 dB. Light generation is achieved via antenna-enhanced inelastic tunneling of electrons over the antenna feed gap. We obtain reproducible tunnel gaps by means of feedback-controlled dielectrophoresis, which precisely places single surface-passivated gold nanoparticles in the antenna gap. The resulting antennas perform equivalent to radio-frequency antennas and combined with waveguiding layers even outperform RF designs. This work paves the way for optical on-chip data communication that is not restricted by Joule heating but also for advanced light management in nanoscale sensing and metrology as well as light emitting devices.
R. Kullock, M. Ochs, P. Grimm & B. Hecht
Nature Comm. 11, 115 (2020)
We use mono-crystalline gold platelets with ultra-smooth surfaces and superior plasmonic properties to investigate the formation of interference patterns caused by surface plasmon polaritons (SPPs) with scattering-type scanning near-field microscopy (s-SNOM) at 521 nm and 633 nm. By applying a Fourier analysis approach, we can identify and separate several signal channels related to SPPs launched and scattered by the AFM tip and the edges of the platelet. Especially at the excitation wavelength of 633 nm, we can isolate a region in the center of the platelets where we find only contributions of SPPs which are launched by the tip and reflected at the edges. These signatures are used to determine the SPP wavelength of lambda_SPP = 606 nm good agreement with theoretical predictions. Furthermore, we were still able to measure SPP signals after 20 μm propagation, which demonstrates impressively the superior plasmonic quality of these mono-crystalline gold platelets.
K.J. Kaltenecker, E. Krauss, L. Casses, M. Geisler, B. Hecht, N.A. Mortensen, P.U. Jepsen & N. Stenger
Nanophotonics 0362 (2019) arxiv:1909.08321 (2019)