arXiv subjects

Martin Wolf

Publications and source records attributed to Martin Wolf.

At least 109 records · Page 6Linked to original sources

arXiv2019

Second Harmonic Generation from Phononic Epsilon-Near-Zero Berreman Modes in Ultrathin Polar Crystal Films

Immense optical field enhancement was predicted to occur for the Berreman mode in ultrathin films at frequencies in the vicinity of epsilon near zero (ENZ). Here, we report the first experimental proof of this prediction in the mid-infrared by probing the resonantly enhanced second harmonic generation (SHG) at the longitudinal optic phonon frequency from a deeply subwavelength-thin aluminum nitride (AlN) film. Employing a transfer matrix formalism, we show that the field enhancement is completely localized inside the AlN layer, revealing that the observed SHG signal of the Berreman mode is solely generated in the AlN film. Our results demonstrate that ENZ Berreman modes in intrinsically low-loss polar dielectric crystals constitute a promising platform for nonlinear nanophotonic applications.

physics.optics↗

arXiv2019

Surface phonon polariton resonance imaging using long-wave infrared-visible sum-frequency generation microscopy

We experimentally demonstrate long-wave infrared-visible sum-frequency generation microscopy for imaging polaritonic resonances of infrared (IR) nanophotonic structures. This nonlinear-optical approach provides direct access to the resonant field enhancement of the polaritonic near fields, while the spatial resolution is limited by the wavelength of the visible sum-frequency signal. As a proof-of-concept, we here study periodic arrays of subdiffractional nanostructures made of 4H-silicon carbide supporting localized surface phonon polaritons. By spatially scanning tightly focused incident beams, we observe excellent sensitivity of the sum-frequency signal to the resonant polaritonic field enhancement, with a much improved spatial resolution determined by visible laser focal size. However, we report that the tight focusing can also induce sample damage, ultimately limiting the achievable resolution with the scanning probe method. As a perspective approach towards overcoming this limitation, we discuss the concept of using wide-field sum-frequency generation microscopy as a universal experimental tool that would offer long-wave IR super-resolution microscopy with spatial resolution far below the IR diffraction limit.

physics.optics↗

arXiv2019

Low-temperature infrared dielectric function of hyperbolic $α$-quartz

We report the infrared dielectric properties of $α$-quartz in the temperature range from $1.5\ \mathrm{K}$ to $200\ \mathrm{K}$. Using an infrared free-electron laser, far-infrared reflectivity spectra of a single crystal $y$-cut were acquired along both principal axes, under two different incidence angles, in S- and P-polarization. These experimental data have been fitted globally for each temperature with a multioscillator model, allowing to extract frequencies and damping rates of the ordinary and extraordinary, transverse and longitudinal optic phonon modes, and hence the temperature-dependent dispersion of the infrared dielectric function. The results are in line with previous high-temperature studies, allowing for a parametrized description of all temperature-dependent phonon parameters and the resulting dielectric function from $1.5\ \mathrm{K}$ up to the $α$-$β$-phase transition temperature, $T_C = 846\ \mathrm{K}$. Using these data, we predict remarkably high quality factors for polaritons in $α$-quartz's hyperbolic spectral region at low temperatures.

cond-mat.mtrl-sci↗

arXiv2019

Revealing the Competing Contributions of Charge Carriers, Excitons, and Defects to the Non-Equilibrium Optical Properties of ZnO

Due to its wide band gap and high carrier mobility, ZnO is an attractive material for light-harvesting and optoelectronic applications. Its functional efficiency, however, is strongly affected by defect-related in-gap states that open up extrinsic decay channels and modify relaxation timescales. As a consequence, almost every ZnO sample behaves differently, leading to irreproducible or even contradicting observations. Here, a complementary set of time-resolved spectroscopies is applied to two ZnO samples of different defect density to disentangle the competing contributions of charge carriers, excitons, and defects to the non-equilibrium dynamics after photoexcitation: Time-resolved photoluminescence, excited state transmission, and electronic sum frequency generation. Remarkably, defects affect the transient optical properties of ZnO across more than eight orders of magnitude in time, starting with photodepletion of normally occupied defect states on femtosecond timescales, followed by the competition of free exciton emission and exciton trapping at defect sites within picoseconds, photoluminescence of defect-bound and free excitons on nanosecond timescales, and deeply trapped holes with microsecond lifetimes. These findings do not only provide the first comprehensive picture of charge and exciton relaxation pathways in ZnO, but also uncover the microscopic origin of previous conflicting observations in this challenging material and thereby offer means of overcoming its difficulties.

cond-mat.mtrl-sci↗

arXiv2019

Higher Structures in M-Theory

The key open problem of string theory remains its non-perturbative completion to M-theory. A decisive hint to its inner workings comes from numerous appearances of higher structures in the limits of M-theory that are already understood, such as higher degree flux fields and their dualities, or the higher algebraic structures governing closed string field theory. These are all controlled by the higher homotopy theory of derived categories, generalised cohomology theories, and $L_\infty$-algebras. This is the introductory chapter to the proceedings of the LMS/EPSRC Durham Symposium on Higher Structures in M-Theory. We first review higher structures as well as their motivation in string theory and beyond. Then we list the contributions in this volume, putting them into context.

hep-th↗

arXiv2019

$L_\infty$-Algebras, the BV Formalism, and Classical Fields

We summarise some of our recent works on $L_\infty$-algebras and quasi-groups with regard to higher principal bundles and their applications in twistor theory and gauge theory. In particular, after a lightning review of $L_\infty$-algebras, we discuss their Maurer-Cartan theory and explain that any classical field theory admitting an action can be reformulated in this context with the help of the Batalin-Vilkovisky formalism. As examples, we explore higher Chern-Simons theory and Yang-Mills theory. We also explain how these ideas can be combined with those of twistor theory to formulate maximally superconformal gauge theories in four and six dimensions by means of $L_\infty$-quasi-isomorphisms, and we propose a twistor space action.

hep-th↗

arXiv2019

Controlling Nanoscale Air-Gaps for Critically Coupled Surface Polaritons by Means of Non-Invasive White-Light Interferometry

We report an experimental method to control large-area air-gaps in the nanometer range for evanescent coupling of light to surface waves such as surface plasmon polaritons or surface phonon polaritons. With the help of spectrally resolved white-light interferometry we are able to stabilize and tune the gap with nanometer precision and high parallelism. Our technique is non-invasive, leaves the coupling area unobstructed, and the setup delivers reference-free real-time readout up to 150 μm distance between the coupling prism and sample. Furthermore, we demonstrate the application to prism coupled surface polariton excitation. The active gap control is used to determine the dispersion of a critically coupled surface phonon polariton over a wide spectral range in the mid infrared.

physics.optics↗

arXiv2018

Beyond the molecular movie: dynamics of bands and bonds during a photo-induced phase transition

Ultrafast non-equilibrium dynamics offer a route to study the microscopic interactions that govern macroscopic behavior. In particular, photo-induced phase transitions (PIPTs) in solids provide a test case for how forces, and the resulting atomic motion along a reaction coordinate, originate from a non-equilibrium population of excited electronic states. Utilizing femtosecond photoemission we obtain access to the transient electronic structure during an ultrafast PIPT in a model system: indium nanowires on a silicon(111) surface. We uncover a detailed reaction pathway, allowing a direct comparison with the dynamics predicted by ab initio simulations. This further reveals the crucial role played by localized photo-holes in shaping the potential energy landscape, and enables a combined momentum and real space description of PIPTs, including the ultrafast formation of chemical bonds.

cond-mat.str-el↗

arXiv2018

Strong Coupling of Epsilon-Near-Zero Phonon Polaritons in Polar Dielectric Heterostructures

We report the first observation of epsilon near zero (ENZ) phonon polaritons in an ultrathin AlN film fully hybridized with surface phonon polaritons (SPhP) supported by the adjacent SiC substrate. Employing a strong coupling model for the analysis of the dispersion and electric field distribution in these hybridized modes, we show that they share the most prominent features of the two precursor modes. The novel ENZ-SPhP coupled polaritons with a highly propagative character and deeply sub-wavelength light confinement can be utilized as building blocks for future infrared and terahertz (THz) nanophotonic integration and communication devices.

physics.optics↗

arXiv2018

Terahertz spectroscopy for all-optical spintronic characterization of the spin-Hall-effect metals Pt, W and Cu$_{80}$Ir$_{20}$

Identifying materials with an efficient spin-to-charge conversion is crucial for future spintronic applications. The spin Hall effect is a central mechanism as it allows for the interconversion of spin and charge currents. Spintronic material research aims at maximizing its efficiency, quantified by the spin Hall angle $Θ_{\textrm{SH}}$ and the spin-current relaxation length $λ_{\textrm{rel}}$. We develop an all-optical method with large sample throughput that allows us to extract $Θ_{\textrm{SH}}$ and $λ_{\textrm{rel}}$. Employing terahertz spectroscopy, we characterize magnetic metallic heterostructures involving Pt, W and Cu$_{80}$Ir$_{20}$ in terms of their optical and spintronic properties. We furthermore find indications that the interface plays a minor role for the spin-current transmission. Our analytical model is validated by the good agreement with literature DC values. These findings establish terahertz emission spectroscopy as a reliable tool complementing the spintronics workbench.

cond-mat.mtrl-sci↗

arXiv2018

Dissecting spin-phonon equilibration in ferrimagnetic insulators by ultrafast lattice excitation

To gain control over magnetic order on ultrafast time scales, a fundamental understanding of the way electron spins interact with the surrounding crystal lattice is required. However, measurement and analysis even of basic collective processes such as spin-phonon equilibration have remained challenging. Here, we directly probe the flow of energy and angular momentum in the model insulating ferrimagnet yttrium iron garnet. Following ultrafast resonant lattice excitation, we observe that magnetic order reduces on distinct time scales of 1 ps and 100 ns. Temperature-dependent measurements, a spin-coupling analysis and simulations show that the two dynamics directly reflect two stages of spin-lattice equilibration. On the 1-ps scale, spins and phonons reach quasi-equilibrium in terms of energy through phonon-induced modulation of the exchange interaction. This mechanism leads to identical demagnetization of the ferrimagnet's two spin-sublattices and a novel ferrimagnetic state of increased temperature yet unchanged total magnetization. Finally, on the much slower, 100-ns scale, the excess of spin angular momentum is released to the crystal lattice, resulting in full equilibrium. Our findings are relevant for all insulating ferrimagnets and indicate that spin manipulation by phonons, including the spin Seebeck effect, can be extended to antiferromagnets and into the terahertz frequency range.

cond-mat.mtrl-sci↗

arXiv2018

Detecting Weak Signals from Interfaces by High Accuracy Phase-Resolved SFG Spectroscopy

Much work over the last 25 years has demonstrated that the interface-specific, alloptical technique, vibrational sum frequency generation (v-SFG) spectroscopy, is often uniquely capable of characterizing the structure and dynamics of interfacial species. The desired information in such a measurement is the complex second order susceptibility which gives rise to the nonlinear response from interfacial molecules. The ability to detect molecular species yielding only small contributions to the susceptibility is meanwhile limited by the precision by which the spectral phase and amplitude can be determined. In this study we describe a new spectrometer design that offers unprecedented phase and amplitude accuracy while significantly improving the sensitivity of the technique. Combining a full collinear beam geometry with a technique enabling the simultaneous measurement of the complex sample and reference spectrum, uncertainties in the reference phase and amplitude are shown to be greatly reduced. Furthermore, we show that using balanced detection, the signal to noise ratio can be increased by one order of magnitude. The capabilities of the spectrometer are demonstrated by the isolation of a small isotropic surface signal from the bulk dominated nonlinear optical response of z-cut quartz. The achieved precision of our spectrometer enables measurements not currently feasible in v-SFG spectroscopy.

physics.optics↗

arXiv2018

Second harmonic generation from strongly coupled localized and propagating phonon-polariton modes

We experimentally investigate second harmonic generation from strongly coupled localized and propagative phonon polariton modes in arrays of silicon carbide nanopillars. Our results clearly demonstrate the hybrid nature of the system's eigenmodes and distinct manifestation of strong coupling in the linear and nonlinear response. While in linear reflectivity the intensity of the two strongly-coupled branches is essentially symmetric and well explained by their respective localized or propagative components, the second harmonic signal presents a strong asymmetry. Analyzing it in detail, we reveal the importance of interference effects between the nonlinear polarization terms originating in the bulk and in the phonon polariton modes, respectively.

cond-mat.mes-hall↗

arXiv2018

Controlling the Infrared Dielectric Function through Atomic-Scale Heterostructures

Surface phonon polaritons (SPhPs) - the surface-bound electromagnetic modes of a polar material resulting from the coupling of light with optic phonons - offer immense technological opportunities for nanophotonics in the infrared (IR) spectral region. Here, we present a novel approach to overcome the major limitation of SPhPs, namely the narrow, material-specific spectral range where SPhPs can be supported, called the Reststrahlen band. We use an atomic-scale superlattice (SL) of two polar semiconductors, GaN and AlN, to create a hybrid material featuring layer thickness-tunable optic phonon modes. As the IR dielectric function is governed by the optic phonon behavior, such control provides a means to create a new dielectric function distinct from either constituent material and to tune the range over which SPhPs can be supported. This work offers the first glimpse of the guiding principles governing the degree to which the dielectric function can be designed using this approach.

cond-mat.mtrl-sci↗

arXiv2018

Direct observation of near-field induced resonant electron tunneling in a sub-nanometer plasmonic gap

Localized surface plasmon resonance (LSPR) excitation of nanostructures and charge transfer in plasmonic nanocavities plays a central role in nanoscale optoelectronics and in applications for plasmonic devices. However, the direct observation of near-filed induced charge transfer has remained as a challenging experiment. Here we present LSPR-assisted resonant electron tunneling from an Ag or Au tip to the image potential states of a Ag(111) surface using scanning tunneling microscopy (STM). The LSPR-assisted tunneling process results in an incident photon-energy dependent red-shift of the field emission resonances (FERs) in the gap. Using the precise control of the gap distance in the STM junction we demonstrate tuning of the relative contribution from the LSPR-assisted and the normal STM electron tunneling processes. Furthermore, the FER intensity mapping of local defects on the surface allows assigning unambiguously the respective FER levels with and without laser excitation.

cond-mat.mes-hall↗

arXiv2018

Second-harmonic phonon spectroscopy of $α$-quartz

We demonstrate midinfrared second-harmonic generation as a highly sensitive phonon spectroscopy technique that we exemplify using $α$-quartz (SiO$_2$) as a model system. A midinfrared free-electron laser provides direct access to optical phonon resonances ranging from $350\ \mathrm{cm}^{-1}$ to $1400\ \mathrm{cm}^{-1}$. While the extremely wide tunability and high peak fields of an free-electron laser promote nonlinear spectroscopic studies---complemented by simultaneous linear reflectivity measurements---azimuthal scans reveal crystallographic symmetry information of the sample. Additionally, temperature-dependent measurements show how damping rates increase, phonon modes shift spectrally and in certain cases disappear completely when approaching $T_c=846\ \mathrm{K}$ where quartz undergoes a structural phase transition from trigonal $α$-quartz to hexagonal $β$-quartz, demonstrating the technique's potential for studies of phase transitions.

cond-mat.mtrl-sci↗

arXiv2017

Experimentally Probing 'Hydrophobic' Water at the Gold Electrode/Aqueous Interface

Quantitative description of reaction mechanisms in aqueous phase electrochemistry requires experimental characterization of local water structure at the electrode/aqueous interface and its evolution with changing potential. Gaining such insight experimentally under electrochemical conditions is a formidable task. Here we characterize the potential dependent structure of a sub-population of interfacial water that have one OH group pointing towards a gold working electrode using interface specific vibrational spectroscopy in a thin film electrochemical cell. Such 'free-OH' groups are the molecular level observable of an extended hydrophobic interface. This 'free-OH' interacts only weakly with the Au surface at all potentials, has an orientational distribution that narrows as one approaches the potential of zero charge and disappears on the oxidation of the gold electrode.

physics.chem-ph↗

arXiv2017

Supersymmetric Yang-Mills Theory as Higher Chern-Simons Theory

We observe that the string field theory actions for the topological sigma models describe higher or categorified Chern-Simons theories. These theories yield dynamical equations for connective structures on higher principal bundles. As a special case, we consider holomorphic higher Chern-Simons theory on the ambitwistor space of four-dimensional space-time. In particular, we propose a higher ambitwistor space action functional for maximally supersymmetric Yang-Mills theory.

hep-th↗