M. Wagner

Tunable Phonon Polaritons in Atomically Thin van der Waals Crystals of Boron Nitride

Nanoimaged Polaritons Engineered heterostructures consisting of thin, weakly bound layers can exhibit many attractive electronic properties. Dai et al. (p. 1125) used infrared nanoimaging on the surface of hexagonal boron nitride crystals to detect phonon polaritons, collective modes that originate in the coupling of photons to optical phonons. The findings reveal the dependence of the polariton wavelength and dispersion on the thickness of the material down to just a few atomic layers. Infrared nanoimaging is used to detect a type of surface collective mode in a representative van der Waals crystal. van der Waals heterostructures assembled from atomically thin crystalline layers of diverse two-dimensional solids are emerging as a new paradigm in the physics of materials. We used infrared nanoimaging to study the properties of surface phonon polaritons in a representative van der Waals crystal, hexagonal boron nitride. We launched, detected, and imaged the polaritonic waves in real space and altered their wavelength by varying the number of crystal layers in our specimens. The measured dispersion of polaritonic waves was shown to be governed by the crystal thickness according to a scaling law that persists down to a few atomic layers. Our results are likely to hold true in other polar van der Waals crystals and may lead to new functionalities.

Local Charge and Spin Currents in Magnetothermal Landscapes

A scannable laser beam is used to generate local thermal gradients in metallic (Co2FeAl) or insulating (Y3Fe5O12) ferromagnetic thin films. We study the resulting local charge and spin currents that arise due to the anomalous Nernst effect (ANE) and the spin Seebeck effect (SSE), respectively. In the local ANE experiments, we detect the voltage in the Co2FeAl thin film plane as a function of the laser-spot position and external magnetic field magnitude and orientation. The local SSE effect is detected in a similar fashion by exploiting the inverse spin Hall effect in a Pt layer deposited on top of the Y3Fe5O12. Our findings establish local thermal spin and charge current generation as well as spin caloritronic domain imaging.

Ultrafast and Nanoscale Plasmonic Phenomena in Exfoliated Graphene Revealed by Infrared Pump–Probe Nanoscopy

Pump-probe spectroscopy is central for exploring ultrafast dynamics of fundamental excitations, collective modes, and energy transfer processes. Typically carried out using conventional diffraction-limited optics, pump-probe experiments inherently average over local chemical, compositional, and electronic inhomogeneities. Here, we circumvent this deficiency and introduce pump-probe infrared spectroscopy with ∼ 20 nm spatial resolution, far below the diffraction limit, which is accomplished using a scattering scanning near-field optical microscope (s-SNOM). This technique allows us to investigate exfoliated graphene single-layers on SiO2 at technologically significant mid-infrared (MIR) frequencies where the local optical conductivity becomes experimentally accessible through the excitation of surface plasmons via the s-SNOM tip. Optical pumping at near-infrared (NIR) frequencies prompts distinct changes in the plasmonic behavior on 200 fs time scales. The origin of the pump-induced, enhanced plasmonic response is identified as an increase in the effective electron temperature up to several thousand Kelvin, as deduced directly from the Drude weight associated with the plasmonic resonances.

Ultrafast Dynamics of Surface Plasmons in InAs by Time-Resolved Infrared Nanospectroscopy

We report on time-resolved mid-infrared (mid-IR) near-field spectroscopy of the narrow bandgap semiconductor InAs. The dominant effect we observed pertains to the dynamics of photoexcited carriers and associated surface plasmons. A novel combination of pump-probe techniques and near-field nanospectroscopy accesses high momentum plasmons and demonstrates efficient, subpicosecond photomodulation of the surface plasmon dispersion with subsequent tens of picoseconds decay under ambient conditions. The photoinduced change of the probe intensity due to plasmons in InAs is found to exceed that of other mid-IR or near-IR media by 1-2 orders of magnitude. Remarkably, the required control pulse fluence is as low as 60 μJ/cm(2), much smaller than fluences of ∼ 1-10 mJ/cm(2) previously utilized in ultrafast control of near-IR plasmonics. These low excitation densities are easily attained with a standard 1.56 μm fiber laser. Thus, InAs--a common semiconductor with favorable plasmonic properties such as a low effective mass--has the potential to become an important building block of optically controlled plasmonic devices operating at infrared frequencies.

Graphene-Based Platform for Infrared Near-Field Nanospectroscopy of Water and Biological Materials in an Aqueous Environment

Scattering scanning near-field optical microscopy (s-SNOM) has emerged as a powerful nanoscale spectroscopic tool capable of characterizing individual biomacromolecules and molecular materials. However, applications of scattering-based near-field techniques in the infrared (IR) to native biosystems still await a solution of how to implement the required aqueous environment. In this work, we demonstrate an IR-compatible liquid cell architecture that enables near-field imaging and nanospectroscopy by taking advantage of the unique properties of graphene. Large-area graphene acts as an impermeable monolayer barrier that allows for nano-IR inspection of underlying molecular materials in liquid. Here, we use s-SNOM to investigate the tobacco mosaic virus (TMV) in water underneath graphene. We resolve individual virus particles and register the amide I and II bands of TMV at ca. 1520 and 1660 cm(-1), respectively, using nanoscale Fourier transform infrared spectroscopy (nano-FTIR). We verify the presence of water in the graphene liquid cell by identifying a spectral feature associated with water absorption at 1610 cm(-1).

Generation and Detection of THz Radiation With Scalable Antennas Based on GaAs Substrates With Different Carrier Lifetimes

We report on scalable photoconductive antennas for both emission and detection of terahertz (THz) radiation. The concept yields THz emitters with high efficiencies for the conversion of near-infrared into far-infrared radiation, and provides detectors that do not require tight focusing of both the THz beam and the near-infrared gating beam. GaAs substrates implanted with dual energy implants of N+ and As+ ions of various doses are compared with semiinsulating (SI) and low-temperature-grown GaAs. We discuss which material properties are desirable for emitters and detectors and identify which material is optimal as either emitter or detector substrate. Best results for detectors are found for implanted samples with doses in the range of 1013 cm-2 for GaAs:N and for LT-GaAs. Best emitters for typical excitation conditions with a Ti: sapphire oscillator system are based on SI-GaAs.

Tunneling Plasmonics in Bilayer Graphene.

We report experimental signatures of plasmonic effects due to electron tunneling between adjacent graphene layers. At subnanometer separation, such layers can form either a strongly coupled bilayer graphene with a Bernal stacking or a weakly coupled double-layer graphene with a random stacking order. Effects due to interlayer tunneling dominate in the former case but are negligible in the latter. We found through infrared nanoimaging that bilayer graphene supports plasmons with a higher degree of confinement compared to single- and double-layer graphene, a direct consequence of interlayer tunneling. Moreover, we were able to shut off plasmons in bilayer graphene through gating within a wide voltage range. Theoretical modeling indicates that such a plasmon-off region is directly linked to a gapped insulating state of bilayer graphene, yet another implication of interlayer tunneling. Our work uncovers essential plasmonic properties in bilayer graphene and suggests a possibility to achieve novel plasmonic functionalities in graphene few-layers.

Simultaneous time and wavelength resolved spectroscopy under two-colour near infrared and terahertz excitation

Time and wavelength resolved spectroscopy requires optical sources emitting very short pulses and a fast detection mechanism capable of measuring the evolution of the output spectrum as a function of time. We use table-top Ti:sapphire lasers and a free-electron laser (FEL) emitting ps pulses as excitation sources and a streak camera coupled to a spectrometer for detection. One of the major aspects of this setup is the synchronization of pulses from the two lasers which we describe in detail. Optical properties of the FEL pulses are studied by autocorrelation and electro-optic sampling measurements. We discuss the advantages of using this setup to perform photoluminescence quenching in semiconductor quantum wells and quantum dots. Carrier redistribution due to pulsed excitation in these heterostructures can be investigated directly. Sideband generation in quantum wells is also studied where the intense FEL pulses facilitate the detection of the otherwise weak nonlinear effect.

Resonant enhancement of second order sideband generation for intraexcitonic transitions in GaAs/AlGaAs multiple quantum wells

We present an experimental study on efficient second order sideband generation in symmetric undoped GaAs/AlGaAs multiple quantum wells. A near-infrared laser tuned to excitonic interband transitions is mixed with an in-plane polarized terahertz beam from a free-electron laser. The terahertz beam is tuned either to the intraexcitonic heavy-hole 1s-2p transition or to the interexcitonic heavy-hole light-hole transition. We find strong evidence that the intraexcitonic transition is of paramount influence on n=±2 sideband generation, leading to an order-of-magnitude resonant enhancement of the conversion efficiency up to 0.1% at low temperature. At room temperature, the efficiency drops only by a factor of 7 for low terahertz powers.

Tunable narrowband THz pulse generation in scalable large area photoconductive antennas

The generation and characterization of narrowband THz pulses by means of chirped pulse difference frequency generation in Auston-switch type photoconductive antennas is reported. Using optical pulses with energies in the range from 1 nJ to 1 µJ, we generate THz pulses with up to 50 pJ in energy and electric field strengths on the order of 1 kV/cm. Two emitter concepts are investigated and circumvention of the fast saturation for small area excitation by scaling of the THz emitter is demonstrated.