Inverse-Designed Narrowband THz Radiator for Ultrarelativistic Electrons

THz radiation finds various applications in science and technology. Pump-probe experiments at free-electron lasers typically rely on THz radiation generated by optical rectification of ultrafast laser pulses in electro-optic crystals. A compact and cost-efficient alternative is offered by the Smith-Purcell effect: a charged particle beam passes a periodic structure and generates synchronous radiation. Here, we employ the technique of photonic inverse design to optimize a structure for Smith-Purcell radiation at a single wavelength from ultrarelativistic electrons. The resulting design is highly resonant and emits narrowbandly. Experiments with a 3D-printed model for a wavelength of 900 mu m show coherent enhancement. The versatility of inverse design offers a simple adaption of the structure to other electron energies or radiation wavelengths. This approach could advance beam-based THz generation for a wide range of applications.

Génération de deuxième et troisième harmonique avec un laser Nd:YAG en régime pulsé libre

Sébastian Favre

Industrial laser precision machining is predominately based on pulsed Nd:YAG lasers operated at a wavelength of 1.06 µm in a free running pulse regime. The objective of this thesis work has been to investigate second and third harmonic generation for such "long pulse" Nd:YAG lasers. Visible and UV radiation can be better focused. The absorption coefficient at these wavelengths is higher in most materials. Processing at the doubled or tripled frequency increases machining precision and allows processing of new classes of materials such as, e.g., high reflective metals or ceramics. Frequency doubling and tripling of Q-switched, modelocked, or CW operated Nd:YAG lasers has been the subject of numerous publications. However, the particular problems associated with the free running pulse regime have not yet been addressed. The generation of harmonics requires a laser source that can deliver radiation with high brightness. A system based on a slab crystal with a beam quality factor of M2 ≈ 1.6 and a power of up to 1.5 kW has been used in the experiments. An external electro-optical switch has been implemented in order to precisely control the laser pulse shape and duration. The non-linear coefficient and the angular acceptance have been the main criteria for selecting LBO (LiB3O5), KTP (KTiOPO4), and MgO:LiNbO3 for the frequency conversion experiments. The conversion efficiency has been measured for these crystals as a function of the intensity at the fundamental wavelength. In contrast to simple model predictions, the efficiency does not increase linearly with intensity under long pulse conditions. An intensity dependant phase mismatch is at the origin of the deviations. A heuristic model for the efficiency prediction has been developed. It is based on a linear increase of phase mismatch with intensity and it allows describing the experimental findings with sufficient accuracy. The conversion efficiency for frequency doubling is limited to about 20% at pulse durations of 100 µsec. It decreases with increasing pulse duration. Catastrophic thermal damage is at the origin of the limitation in this pulse regime. Our experiments indicate that the damage is initiated by the frequency doubled light. Temporary color centers are created in the presence of the second harmonic light. The dynamic of the creation and annihilation of these centers has been investigated. It could be shown that finally the absorption of the fundamental harmonic (infrared) radiation at these centers results in irreversible thermal damages. A power of 140 W in the second harmonic (178 MW/cm2 on a waist of 5 µm) and 12 W in the third harmonic (61 MW/cm2 in a waist of 2.5 µm) was obtained with pulses of 200 µs. This allowed to demonstrate the feasibility of material processing with very high reproducibility and definition, which for instance allowed the design and the manufacturing of micro-grippers and several other prototypes in the field of robotics and micro-engineering.

EPFL2001

Electronic and vibrational spectroscopy of cold protonated amino acids in the gas phase

Sébastien Mercier

In this thesis report, we describe a novel home-built instrument designed to study the spectroscopy of biomolecular ions in the gas phase and at low temperature, and we present the first experimental results obtained on protonated aromatic amino acids. The apparatus consists in a tandem mass spectrometer equipped with a nanospray ion source and a cryocooled 22-pole ion trap. The charged species produced by the source traverse a first quadrupole mass filter and mass-selected ions are then accumulated and thermalized in the ion trap, where their vibrational temperature can be lowered to ~ 10 K. Two setups allow us to generate ultraviolet and infrared laser light to spectroscopically probe the trapped ions by photodissociation. The resulting fragment ions are finally released from the trap and mass analyzed by a second quadrupole spectrometer. Photodissociation electronic spectra have been measured for the protonated amino acids tryptophan (TrpH+) and tyrosine (TyrH+), as well as for hydrated complexes of the former. The spectrum of TyrH+ exhibits sharp, fully resolved vibronic transitions, which attests to the low temperature of the ions. In contrast, that of tryptophan shows a broad absorption band that covers several hundreds of wavenumbers. This has been attributed to lifetime broadening related to an ultrafast (< ~ 100 fs) deactivation mechanism of the TrpH+ S1(ππ*) excited state. This phenomenon is caused by a strong coupling between this ππ* state and a nearby dissociative state of πσ* character mainly localized on the charged ammonium group. Solvation of TrpH+ by only two water molecules is sufficient to significantly destabilize the σ* orbitals and reduce that coupling, which results in a longer excited-state lifetime and a fully resolved electronic spectrum. These interpretations are supported by ab initio and density functional theory (DFT) calculations. Infrared-ultraviolet double resonance spectroscopic techniques have been successfully implemented to identify the different conformers of TyrH+ and doubly hydrated protonated tryptophan (TrpH+·W2) by measuring conformer-specific vibrational and electronic spectra for each of them. By comparison with the results of DFT geometry and harmonic frequency calculations, we could confidently determine the structures of the TyrH+ conformers and suggest possible assignments for those of TrpH+·W2. Two important stabilizing interactions could be inferred from these results: (i) the attraction between the charged ammonium group and the π-electron cloud of the aromatic ring; (ii) the hydrogen-bonding interaction of a donor water molecule to the acceptor indole ring of TrpH+·W2.

EPFL2008

Intrinsic Emittance Reduction of an Electron Beam from Metal Photocathodes

Christoph Peter Hauri

Electron beams in modern linear accelerators are now becoming limited in brightness by the intrinsic emittance of the photocathode electron source. Therefore it becomes important for large scale facilities such as free electron lasers to reduce this fundamental limit. In this Letter we present measurements of the intrinsic emittance for different laser wavelength (from 261 to 282 nm) and for different photocathode materials such as Mo, Nb, Al, Cu. Values as low as 0.41±0.03mm•mrad/mm laser spot size (rms) were measured for a copper photocathode illuminated with a 282 nm laser wavelength. The key element for emittance reduction is a uv laser system which allows adjustment of the laser photon energy to match the effective work function of the cathode material and to emit photoelectrons with a lower initial kinetic energy. The quantum efficiency over the explored wavelength range varies by less than a factor of 3. © 2010 The American Physical Society.