Ultrafast spectroscopy allows us to probe and understand material properties. With it, we can measure phonon-polaritons (optical phonons coupled with light) and the resulting dispersion curve in lithium niobate. Customizing the excitation source in ultrafast measurements can excite phonon modes to large amplitudes, allowing the experimental exploration of the Potential Energy Surface in solids. However, stronger pump fluences and bigger signal isn't always the answer in ultrafast spectroscopy. When sample signals and their nonlinear and mechanisms cannot be distinguished with 1D measurements, simple 2D THz measurements are a great place to start searching for distinct factors as was the case in cadmium tungstate. 2D measurements when paired with modeling and first principles calculations can reveal cutting edge information about exciting materials.

Terahertz (THz)-band communication is envisioned as a critical technology that could satisfy the need for much higher data rates in sixth generation wireless communi- cation (6G) systems and beyond. Although THz signal propagation suffers from huge spreading and molecular absorption losses that limit the achievable commu- nication ranges, ultra-massive multiple-input multiple-output (UM-MIMO) antenna arrays can introduce the required beamforming gains to compensate for these losses. The reconfigurable UM-MIMO systems of small footprints motivate the use of spatial modulation techniques. Furthermore, the ultra-wideband fragmented THz spectrum motivates the use of index modulation techniques over multicarrier channels. In this thesis, we consider the problem of efficient index mapping and data detection in THz- band index modulation paradigms. We first propose an accurate frequency-domain statistical UM-MIMO channel model for wideband multicarrier THz-band commu- nications by considering THz-specific features. We then propose several THz-band generalized index modulation schemes that provide various performance and complex- ity tradeoffs. We propose efficient algorithms for mapping information bits to antenna and frequency indices at the transmitter side to enhance the achievable data rates in THz channel uses. We further propose complementary low-complexity parameter estimation and data detection techniques at the receiver side that can scale efficiently with very high rates. We derive theoretical bounds on the achievable performance gains of the proposed solutions and generate extensive numerical results promoting the corresponding future 6G use cases.

Time-domain terahertz spectroscopy (THz-TDS) is a valuable technique for studying collective ultrafast phenomena. Several mechanisms exist for converting ultrashort optical laser pulses into coherent THz sources. Broadband THz pulses can be obtained from electron currents in air plasma, which requires combinations of different colors of light to be most effective. I report multi-color generation schemes of THz pulses that deliver coherent THz output. Experimental and theoretical work using the photocurrent model describe ways to use non-harmonic color combinations to utilize several sources of light available in a table-top laser setup. Additionally, THz-TDS is used to study a variety of ultrafast electronic phenomena. I describe measurements of THz induced conductivity in high-speed semiconductors, discussed with carrier generation and carrier mobility mechanisms.

This dissertation reports on data acquisition method and the application of world’s first cryogenic apertureless near-field microscope designed for terahertz frequencies. The dissertation briefly summarizes the commonly used data acquisition methods and the existing challenges in applying near-field technology using broadband terahertz sources. We devised, implemented, and validated a novel measurement technique to resolve the challenges. The novel method improves the traditional method by providing the information of the carrier-envelop-phase of the terahertz pulse. The physical properties of WTe₂ microcrystals depend sensitively on the layer number. By applying both the traditional and the novel techniques, we systematically explored the layer-dependent electromagnetic response of mono-layer and few-layer tungsten ditelluride (WTe₂ microcrystals. On tri-layer WTe₂, we discovered the plasmonic response and imaged the real-space pattern of the terahertz plasmon using the novel measurement technique. On bi-layer WTe₂, our measurements support that the band alignment is semi-metallic instead of semi-conducting. Near-field technology at terahertz frequency is sensitive to the Drude behavior of condensed matters. We imaged the electromagnetic response of the transition of cadmium osmate (Cd₂Os₂O₇) crystals from a high temperature metal to a low temperature magnetic insulator. The result is consistent with the temperature dependence in the direct-current conductivity. In the end, the dissertation discusses the theory and simulation of imaging hydrodynamic flow of materials with viscous electron systems via nano-photocurrent technique. In anisotropic material, nano-photocurrent measures the geometrical properties of the Shockley-Ramo auxiliary field or flux. As a result, the nano-photocurrent is a good candidate to detect the boundary layer and vortex flow pattern of a viscous electron system.

No description available.

No / The terahertz frequency spectrum of pentaerythritol tetranitrate (PETN) is calculated using Discover[1] with the COMPASS[2] force field, CASTEP[3] and PWscf.[4] The calculations are compared to each other and to terahertz spectra (0.3-3 THz) of crystalline PETN recorded at 4 K. A number of analysis methods are used to characterise the calculated normal modes.

No / This letter investigates the feasibility of designing a high gain on-chip antenna on silicon technology for subterahertz applications over a wide-frequency range. High gain is achieved by exciting the antenna using an aperture fed mechanism to couple electromagnetics energy from a metal slot line, which is sandwiched between the silicon and polycarbonate substrates, to a 15-element array comprising circular and rectangular radiation patches fabricated on the top surface of the polycarbonate layer. An open ended microstrip line, which is orthogonal to the metal slot-line, is implemented on the underside of the silicon substrate. When the open ended microstrip line is excited it couples the signal to the metal slot-line which is subsequently coupled and radiated by the patch array. Measured results show the proposed on-chip antenna exhibits a reflection coefficient of less than-10 dB across 0.290-0.316 THz with a highest gain and radiation efficiency of 11.71 dBi and 70.8%, respectively, occurred at 0.3 THz. The antenna has a narrow stopband between 0.292 and 0.294 THz. The physical size of the presented subterahertz on-chip antenna is 20 × 3.5 × 0.126 mm3.

No description available.

Ce travail de cette thèse porte sur la dynamique des protéines, accompagnées de leur eau d'hydratation, une couche de solvant autour des protéines vitale pour leur fonction biologique. Chacune de ces deux composantes s'accompagne d'une dynamique qui lui est propre et dont la réunion reforme le paysage énergétique du système biologiquement actif. La mise en application conjointe de la deutération sélective, de la diffusion incohérente de neutrons ainsi que la spectroscopie terahertz a permis d'explorer de manière indépendante la dynamique des protéines et de celles des couches d'hydratation. L'influence de l'état de repliement de la protéine sur sa dynamique a été étudié par diffusion élastique de neutrons. Les protéines globulaires se sont montrées moins dynamiques que ses analogues intrinsèquement désordonnées. Eux même semblent être plus rigides que les protéines dépliées non physiologiques. L'état d'oligomérisation et les conséquences sur la dynamique de ces protéines ont été développés. Les agrégats d'une protéine globulaire se sont avérés être plus flexibles que la forme soluble. A l'inverse, les agrégats d'une protéine désordonnée voient leur dynamique moyenne baisser par rapport à la forme soluble. Ces observations témoignent de la grande diversité de dynamiques à travers le protéome. Les expériences de diffusion incohérente de neutrons sur les couches d'hydratation des protéines globulaires et désordonnées ont permis d'obtenir des informations sur la nature des mouvements de l'eau autour des protéines. Les mesures ont mis en évidence la présence de mouvements translationnels concomitants à l'apparition de la transition dynamique dans les couches d'hydratations, vers 220 K. Les mesures ont de même montré un couplage plus fort entre une protéine désordonnée et son eau d'hydratation que celui entre une protéine globulaire et son eau d'hydratation. La nature de la couche d'hydratation et son influence sur sa dynamique ont été explorés, avec l'utilisation de polymères qui miment le comportement de l'eau et agissent comme source de flexibilité pour la protéine. Pour terminer, la dynamique des groupements méthyles, impliqués dans les modifications dynamiques observées à 150 et 220 K, a été étudiée. / This thesis work focused on the dynamics of proteins, surrounded by their hydration layer, a water shell around the protein vital for its biological function. Each of these components is accompanied by a specific dynamics which union reforms the complex energy landscape of the system. The joint implementation of selective deuteration, incoherent neutron scattering and terahertz spectroscopy allowed to explore the dynamics of proteins and that of the hydration shell. The influence of the folding state of protein on its dynamics has been studied by elastic neutron scattering. Globular proteins were less dynamic than its intrinsically disordered analogues. Themselves appear to be stiffer than non physiological unfolded proteins. The oligomerization state and the consequences on the dynamics were investigated. Aggregates of a globular protein proved to be more flexible than the soluble form. In contrast, aggregates of a disordered protein showed lower average dynamics compared to the soluble form. These observations demonstrate the wide range of dynamics among the proteome. Incoherent neutron scattering experiences on the hydration layer of globular and disordered proteins have yielded information on the nature of water motion around these proteins. The measurements revealed the presence of translational motions concomitant with the onset of the transition dynamics of hydration layers, at 220 K. Measurements have also shown a stronger coupling between a disordered protein and its hydration water, compared to a globular protein and its hydration shell. The nature of the hydration layer and its influence on its dynamics has been explored with the use of polymers that mimic the water behavior and that act as a source of flexibility for the protein. Eventually, the dynamics of methyl groups involved in the dynamical changes observed at 150 and 220 K, was investigated.

In the past decades, the miniaturization in optics led to new devices with structural sizes in the range of the light wavelength, where the photonic modes are con- fined and the number of states is limited. In the smallest microcavities, i.e. micrometer sized optical resonators, the propagation of only one mode is permitted that is simultaneously amplified internally. This particularly strong enhancement of the electric field is directly related to the quality factor of the cavity. By introducing an optical dipole into a high-Q microcavity, the spontaneous emission is amplified at the cavity mode frequency enabling stimulated emission in an inverted system. Although some of theses cavity e®ects can only be understood by quantum elec- trodynamic theory, most mechanisms are accessible by classical and semi-classical approaches. In this thesis, one-dimensional planar microcavities with quality factors up to 4500 have been fabricated by physical vapor deposition of dielectric thin films and organic active materials. A new cavity design based on anisotropic dielectric mirrors grown by oblique angle deposition microcavities with two energetically shifted orthogonally polarized modes is presented. The application of these anisotropic structures for terahertz di®erence signal generation is demonstrated in spectrally and time resolved transmission experiments, where optical beats with repetition rates in the terahertz range are observed. Optically pumped organic vertical cavity surface emitting lasers (VCSELs) have been realized by applying an organic solid state laser compound and high reflectance distributed Bragg reflectors. These lasers combine a very low laser threshold with small beam divergence and good stability. A transfer of the anisotropic design towards an organic VCSEL results in the generation of two perpendicularly polarized laser modes with a splitting adjustable by the fabrication conditions. The observation of an oscillation of two laser modes in a photomixing experiment proves a phase coupling mechanism. This demonstrates the potential of the anisotropic cavity design for a passive or active component in a terahertz radiation source or frequency generator. Furthermore, microcavities with two and three coupled resonators are investigated. By the application of time-resolved transmission experiments, spatial oscil- lations of the internal electric field - photonic Bloch oscillations - are successfully demonstrated. In combination with the anisotropic microcavities, this is a second concept for the modulation of transmitted light with terahertz frequencies. All experiments are accompanied by numerical or analytical models. Transmission experiments of continuously incident light and single laser pulses are compared with transfer matrix simulations and Fourier transform based approaches. For the modeling of emission experiments, a plane wave expansion method is successfully used. For the analysis of the organic VCSEL dynamics, we apply a set of rate equations that explains the gain switching process.