Bernd Metzger

Interpreting Chiral Nanophotonic Spectra: The Plasmonic Born–Kuhn Model

One of the most intuitive ways to classically understand the generation of natural optical activity in chiral media is provided by the coupled oscillator model of Born and Kuhn consisting of two identical, vertically displaced, coupled oscillators. We experimentally realize and discuss its exact plasmonic analog in a system of corner-stacked gold nanorods. In particular, we analyze the arising circular dichroism and optical rotatory spectra in terms of hybridized electromagnetic modes and retardation. Specifically, we demonstrate how tuning the vertical distance between the nanorods can lead to a selective excitation of the occurring bonding and antibonding chiral plasmonic modes.

Doubling the Efficiency of Third Harmonic Generation by Positioning ITO Nanocrystals into the Hot-Spot of Plasmonic Gap-Antennas

We incorporate dielectric indium tin oxide nanocrystals into the hot-spot of gold nanogap-antennas and perform third harmonic spectroscopy on these hybrid nanostructure arrays. The combined system shows a 2-fold increase of the radiated third harmonic intensity when compared to bare gold antennas. In order to identify the origin of the enhanced nonlinear response we perform finite element simulations of the nanostructures, which are in excellent agreement with our measurements. We find that the third harmonic signal enhancement is mainly related to changes in the linear optical properties of the plasmonic antenna resonances when the ITO nanocrystals are incorporated. Furthermore, the dominant source of the third harmonic is found to be located in the gold volume of the plasmonic antennas.

Third Harmonic Mechanism in Complex Plasmonic Fano Structures

We perform third harmonic spectroscopy of dolmen-type nanostructures, which exhibit plasmonic Fano resonances in the near-infrared. Strong third harmonic emission is predominantly radiated close to the low energy peak of the Fano resonance. Furthermore, we find that the third harmonic polarization of the subradiant mode interferes destructively and diminishes the nonlinear signal in the far-field. By comparing the experimental third harmonic spectra with finite element simulations and an anharmonic oscillator model, we find strong indications that the source of the third harmonic is the optical nonlinearity of the bare gold enhanced by the resonant plasmonic polarization.

Strong Enhancement of Second Harmonic Emission by Plasmonic Resonances at the Second Harmonic Wavelength

We perform second harmonic spectroscopy of aluminum nanoantenna arrays that exhibit plasmonic resonances at the second harmonic wavelength between 450 and 570 nm by focusing sub-30 fs laser pulses tunable from 900 to 1140 nm onto the nanoantenna arrays. We find that a plasmonic resonance at the second harmonic wavelength boosts the overall nonlinear process by more than an order of magnitude. In particular, in the measurement the resonant second harmonic polarization component is a factor of about 70 stronger when compared to the perpendicular off-resonant second harmonic polarization. Furthermore, the maximum of the second harmonic conversion efficiency is found to be slightly blue-shifted with respect to the peak of the linear optical far-field spectrum. This fact can be understood from a simple model that accounts for the almost off-resonant absorption at the fundamental wavelength and the resonant emission process at the second harmonic.

Plasmonic Diastereomers: Adding up Chiral Centers

We construct chiral plasmonic molecules by assembling two individual chiral centers. Interestingly, depending on the exact arrangement of the centers, all combinations result in a chiral compound with a strong chiral optical response. Furthermore, we demonstrate that the overall circular dichrosim (CD) is determined by the response of the individual chiral centers. We find that the CD spectra of the composite molecules are then simply given as the sum of the CD spectra of the constituting building blocks. Interestingly, as soon as strong near-field coupling takes place between chiral centers, we find strong deviation from the simple additive chiral behavior. Most importantly, we demonstrate that the optical response of complex chiral plasmonic systems can be decomposed and understood in terms of fundamental building blocks, offering simple and straightforward design rules for future applications such as chiral optical elements and enantiomer sensors.

Nonlinear Plasmonic Sensing

We introduce the concept of nonlinear plasmonic sensing, relying on third harmonic generation from simple plasmonic nanoantennas. Because of the nonlinear conversion process we observe a larger sensitivity to a local change in the refractive index as compared to the commonly used linear localized surface plasmon resonance sensing. Refractive index changes as small as 10(-3) can be detected. In order to determine the spectral position of highest sensitivity, we perform linear and third harmonic spectroscopy on plasmonic nanoantenna arrays, which are the fundamental building blocks of our sensor. Furthermore, simultaneous detection of linear and nonlinear signals allows quantitative comparison of both methods, providing further insight into the working principle of our sensor. While the signal-to-noise ratio is comparable, nonlinear sensing gives about seven times higher relative signal changes.

High-power widely tunable sub-20fs Gaussian laser pulses for ultrafast nonlinear spectroscopy

We demonstrate the generation of widely tunable sub-20 fs Gaussian-shaped laser pulses using a grating-based 4-f pulse shaper and a liquid crystal spatial light modulator. Our pump source is an Yb:KGW solitary mode-locked oscillator at 44 MHz repetition rate which is coupled into a large mode area microstructured fiber to generate a broad spectrum from below 900 nm to above 1150 nm. These pulses are precompressed by a prism sequence and subsequently sent into the pulse shaper. We use the multiphoton intrapulse interference phase scan (MIIPS) for phase shaping and iterative amplitude optimization to achieve Gaussian-like tunable sub-20 fs pulses with output powers of up to 142 mW as well as nontunable pulses with 310 mW output power as short as 11.5 fs.

Nonlinear Refractory Plasmonics with Titanium Nitride Nanoantennas

Titanium nitride (TiN) is a novel refractory plasmonic material which can sustain high temperatures and exhibits large optical nonlinearities, potentially opening the door for high-power nonlinear plasmonic applications. We fabricate TiN nanoantenna arrays with plasmonic resonances tunable in the range of about 950-1050 nm by changing the antenna length. We present second-harmonic (SH) spectroscopy of TiN nanoantenna arrays, which is analyzed using a nonlinear oscillator model with a wavelength-dependent second-order response from the material itself. Furthermore, characterization of the robustness upon strong laser illumination confirms that the TiN antennas are able to endure laser irradiation with high peak intensity up to 15 GW/cm(2) without changing their optical properties and their physical appearance. They outperform gold antennas by one order of magnitude regarding laser power sustainability. Thus, TiN nanoantennas could serve as promising candidates for high-power/high-temperature applications such as coherent nonlinear converters and local heat sources on the nanoscale.

Compact laser source for high-power white-light and widely tunable sub 65 fs laser pulses

We demonstrate an Yb:KGW femtosecond solitary mode-locked laser oscillator, which is used as a pump source for tapered fibers to generate white-light laser pulses with an average output power of up to 2.5 W and a spectral bandwidth of over 1000 nm. By spectrally filtering these pulses and subsequent compression of the filtered pulses with a prism sequence, we are able to generate ultrashort laser pulses with durations between 26 and 65 fs that are tunable from 600 to 1450 nm and with tens to several hundreds of milliwatts of average power.

Probing the Near-Field of Second-Harmonic Light around Plasmonic Nanoantennas

We introduce a new concept that enables subwavelength polarization-resolved probing of the second-harmonic near-field distribution of plasmonic nanostructures. As a local sensor, this method utilizes aluminum nanoantennas, which are resonant to the second-harmonic wavelength and which allow to efficiently scatter the local second-harmonic light to the far-field. We place these sensors into the second-harmonic near-field generated by plasmonic nanostructures and carefully vary their position and orientation. Observing the second-harmonic light resonantly scattered by the aluminum nanoantennas provides polarization-resolved information about the local second-harmonic near-field distribution. We then investigate the polarization-resolved second-harmonic near-field of inversion symmetric gold dipole nanoantennas. Interestingly, we find strong evidence that the second-harmonic dipole is predominantly oriented perpendicular to the gold nanoantenna long axis, although the excitation laser is polarized parallel to the nanoantennas. We believe that our investigations will help to disentangle the highly debated origin of the second-harmonic response of inversion symmetric plasmonic structures. Furthermore, we believe that our new method, which enables the measurement of local nonlinear electric fields, will find widespread implementation and applications in nonlinear near-field optical microscopy.