Valeria Giliberti

Observation of Dirac plasmons in a topological insulator

Plasmons are quantized collective oscillations of electrons and have been observed in metals and doped semiconductors. The plasmons of ordinary, massive electrons have been the basic ingredients of research in plasmonics and in optical metamaterials for a long time. However, plasmons of massless Dirac electrons have only recently been observed in graphene, a purely two-dimensional electron system. Their properties are promising for novel tunable plasmonic metamaterials in the terahertz and mid-infrared frequency range. Dirac fermions also occur in the two-dimensional electron gas that forms at the surface of topological insulators as a result of the strong spin-orbit interaction existing in the insulating bulk phase. One may therefore look for their collective excitations using infrared spectroscopy. Here we report the first experimental evidence of plasmonic excitations in a topological insulator (Bi2Se3). The material was prepared in thin micro-ribbon arrays of different widths W and periods 2W to select suitable values of the plasmon wavevector k. The linewidth of the plasmon was found to remain nearly constant at temperatures between 6 K and 300 K, as expected when exciting topological carriers. Moreover, by changing W and measuring the plasmon frequency in the terahertz range versus k we show, without using any fitting parameter, that the dispersion curve agrees quantitatively with that predicted for Dirac plasmons.

Tunability of the dielectric function of heavily doped germanium thin films for mid-infrared plasmonics

Heavily-doped semiconductor films are very promising for application in mid-infrared plasmonic devices because the real part of their dielectric function is negative and broadly tunable in this wavelength range. In this work we investigate heavily n-type doped germanium epilayers grown on different substrates, in-situ doped in the 10 to 10 cm range, by infrared spectroscopy, first principle calculations, pump-probe spectroscopy and dc transport measurements to determine the relation between plasma edge and carrier density and to quantify mid-infrared plasmon losses. We demonstrate that the unscreened plasma frequency can be tuned in the 400 4800 cm range and that the average electron scattering rate, dominated by scattering with optical phonons and charged impurities, increases almost linearly with frequency. We also found weak dependence of losses and tunability on the crystal defect density, on the inactivated dopant density and on the temperature down to 10 K. In films where the plasma was optically activated by pumping in the near-infrared, we found weak but significant dependence of relaxation times on the static doping level of the film. Our results suggest that plasmon decay times in the several-picosecond range can be obtained in ntype germanium thin films grown on silicon substrates hence allowing for underdamped mid-infrared plasma oscillations at room temperature.

Mapping the amide I absorption in single bacteria and mammalian cells with resonant infrared nanospectroscopy

Infrared (IR) nanospectroscopy performed in conjunction with atomic force microscopy (AFM) is a novel, label-free spectroscopic technique that meets the increasing request for nano-imaging tools with chemical specificity in the field of life sciences. In the novel resonant version of AFM-IR, a mid-IR wavelength-tunable quantum cascade laser illuminates the sample below an AFM tip working in contact mode, and the repetition rate of the mid-IR pulses matches the cantilever mechanical resonance frequency. The AFM-IR signal is the amplitude of the cantilever oscillations driven by the thermal expansion of the sample after absorption of mid-IR radiation. Using purposely nanofabricated polymer samples, here we demonstrate that the AFM-IR signal increases linearly with the sample thickness t for t > 50 nm, as expected from the thermal expansion model of the sample volume below the AFM tip. We then show the capability of the apparatus to derive information on the protein distribution in single cells through mapping of the AFM-IR signal related to the amide-I mid-IR absorption band at 1660 cm(-1). In Escherichia Coli bacteria we see how the topography changes, observed when the cell hosts a protein over-expression plasmid, are correlated with the amide I signal intensity. In human HeLa cells we obtain evidence that the protein distribution in the cytoplasm and in the nucleus is uneven, with a lateral resolution better than 100 nm.

Terahertz current oscillations in a gated two-dimensional electron gas with antenna integrated at the channel ends

We studied terahertz current oscillations induced by a frequency-tunable radiation source in a AlGaAs/InGaAs/AlGaAs heterostructure field effect transistor channel. A planar antenna was integrated on-chip, and a substrate lens was used for broadband coupling of free-space radiation at 0.18–0.72 THz to the channel ends. Through spectral analysis of the detection signal, we identified two different mixing mechanisms: one related to channel current oscillations and the other to modulation of the gate-to-channel potential. Depending on gate bias and radiation frequency, the two mechanisms either compete or cooperate, leading to responsivity up to 300 V/W and noise equivalent power of 1 nW/Hz0.5

Group-IV midinfrared plasmonics

Abstract. The use of heavily doped semiconductors to achieve plasma frequencies in the mid-IR has been recently proposed as a promising way to obtain high-quality and tunable plasmonic materials. We introduce a plasmonic platform based on epitaxial n-type Ge grown on standard Si wafers by means of low-energy plasma-enhanced chemical vapor deposition. Due to the large carrier concentration achieved with P dopants and to the compatibility with the existing CMOS technology, SiGe plasmonics hold promises for mid-IR applications in optoelectronics, IR detection, sensing, and light harvesting. As a representative example, we show simulations of mid-IR plasmonic waveguides based on the experimentally retrieved dielectric constants of the grown materials.

Mapping the electromagnetic field confinement in the gap of germanium nanoantennas with plasma wavelength of 4.5 micrometers

We study plasmonic nanoantennas for molecular sensing in the mid-infrared made of heavily doped germanium, epitaxially grown with a bottom-up doping process and featuring free carrier density in excess of 1020 cm−3. The dielectric function of the 250 nm thick germanium film is determined, and bow-tie antennas are designed, fabricated, and embedded in a polymer. By using a near-field photoexpansion mapping technique at λ = 5.8 μm, we demonstrate the existence in the antenna gap of an electromagnetic energy density hotspot of diameter below 100 nm and confinement volume 105 times smaller than λ3.

Epicatechin-induced conformational changes in β-lactoglobulin B monitored by FT-IR spectroscopy

The interaction between whey carrier protein β-lactoglobulin B and (-)-epicatechin, a major dietary flavonoid with a wide range of health-promoting biological activities, was investigated by Fourier transform infrared spectroscopy in physiological conditions. Amide I spectra of epicatechin - β-lactoglobulin complexes, in D2O buffer solutions, pD= 6.8, at molar ratios from 0.5:1 to 15:1, were measured by using a cell device specifically created. Changes in secondary structure elements at increasing epicatechin concentrations were quantified. Two different trends were observed for the intensities of β-sheet, random coil, and side chain contributions.At molar ratios ≤2 the β-exposed strand contributions (1625 cm−1) increased at the expence of the β-antiparallel sheet band (1637 cm−1). At molar ratios >2 the intensities of both β structures slightly decreased. The same behaviour was observed for the side chain contributions (band around 1610 ÷ 1620 cm−1). In addition, a conformational transition to a slightly opened structure, followed by aggregate formation at the highest molar ratios, were revealed. The results suggest that binding of epicatechin to β-lactoglobulin in physiological conditions occurs at the surface of the protein molecule, resulting in protein dissociation at molar ratios ≤2 with minor changes in secondary structure. This finding provides further evidence for the possibility of successful use of the protein as a carrier of flavonoids, epicatechin included.

Protein clustering in chemically stressed HeLa cells studied by infrared nanospectroscopy

Photo-Thermal Induced Resonance (PTIR) nanospectroscopy, tuned towards amide-I absorption, was used to study the distribution of proteic material in 34 different HeLa cells, of which 18 were chemically stressed by oxidative stress with Na3AsO3. The cell nucleus was found to provide a weaker amide-I signal than the surrounding cytoplasm, while the strongest PTIR signal comes from the perinuclear region. AFM topography shows that the cells exposed to oxidative stress undergo a volume reduction with respect to the control cells, through an accumulation of the proteic material around and above the nucleus. This is confirmed by the PTIR maps of the cytoplasm, where the pixels providing a high amide-I signal were identified with a space resolution of ∼300 × 300 nm. By analyzing their distribution with two different statistical procedures we found that the probability to find protein clusters smaller than 0.6 μm in the cytoplasm of stressed HeLa cells is higher by 35% than in the control cells. These results indicate that it is possible to study proteic clustering within single cells by label-free optical nanospectroscopy.

Heterodyne and subharmonic mixing at 0.6 THz in an AlGaAs/InGaAs/AlGaAs heterostructure field effect transistor

We fabricated a two-dimensional-electron-gas field effect transistor with an asymmetric terahertz antenna connected to the channel terminals and a gate length of 1 μm. We investigated frequency mixing in the transistors channel by measuring, with a quasi-optical setup, the heterodyne, second- and third-order subharmonic mixing signal at 0.592 THz. The dependence on the gate voltage and on the radiation power of both the local-oscillator and the radio-frequency signals was studied for all mixing orders. The conditions for full-plasmonic-mixing are fulfilled in our transistor at room temperature.

Heterogeneity of the Transmembrane Protein Conformation in Purple Membranes Identified by Infrared Nanospectroscopy

Cell membranes are intrinsically heterogeneous, as the local protein and lipid distribution is critical to physiological processes. Even in template systems embedding a single protein type, like purple membranes, there can be a different local response to external stimuli or environmental factors, resulting in heterogeneous conformational changes. Despite the dramatic advances of microspectroscopy techniques, the identification of the conformation heterogeneity is still a challenging task. Tip-enhanced infrared nanospectroscopy is here used to identify conformational changes connected to the hydration state of the transmembrane proteins contained in a 50 nm diameter cell membrane area, without the need for fluorescent labels. In dried purple membrane monolayers, areas with fully hydrated proteins are found among large numbers of molecules with randomly distributed hydration states. Infrared nanospectroscopy results are compared to the spectra obtained with diffraction-limited infrared techniques based on the use of synchrotron radiation, in which the diffraction limit still prevents the observation of nanoscale heterogeneity.