Structured light for ultrafast laser micro- and nanoprocessing
Daniel Flamm, Daniel Günther Grossmann, Marc Sailer, Myriam Kaiser, Felix Zimmermann, Keyou Chen, Michael Jenne, Jonas Kleiner, Julian Hellstern, Christoph Till… 展开作者
Daniel Flamm, Daniel Günther Grossmann, Marc Sailer, Myriam Kaiser, Felix Zimmermann, Keyou Chen, Michael Jenne, Jonas Kleiner, Julian Hellstern, Christoph Tillkorn, Dirk H Sutter, Malte Kumkar
备注：
Accepted manuscript, 19 pages, 20 figures and 111 references
The industrial maturity of ultrashort pulsed lasers has triggered the development of a plethora of material processing strategies. Recently, the combination of these remarkable temporal pulse properties with advanced structured light concepts has led to breakthroughs in the development of novel laser application methods, which will now gradually reach industrial environments. We review the efficient generation of customized focus distributions from the near infrared down to the deep ultraviolet, e.g., based on non-diffracting beams and 3D-beam splitters, and demonstrate their impact for micro- and nanomachining of a wide range of materials. In the beam shaping concepts presented, special attention was paid to suitability for both high energies and high powers.
Ultrafast lasers are ideal tools to process transparent materials because they spatially confine the deposition of laser energy within the material's bulk via nonlinear photoionization processes. Nonlinear propagation and filamentation were initially regarded as deleterious effects. But in the last decade, they turned out to be benefits to control energy deposition over long distances. These effects create very high aspect ratio structures which have found a number of important applications, particularly for glass separation with non-ablative techniques. This chapter reviews the developments o…
Quill effect, one of the intriguing phenomena in ultrafast laser writing, to our knowledge, has not been studied in low-loss-waveguide (LLW) writing regime yet, probably due to its invisibility under conventional white-light microscope in that regime. In this report, with help of adaptive third harmonic generation microscopy we reveal the quill effect in LLW writing regime and study its influences on the properties of written photonic integrated components in term of polarization-related properties in fused silica and beam-splitting ratio of three-waveguide-coupler in borosilicate glass.
All-optical devices are essential for next generation ultrafast, ultralow-power and ultrahigh bandwidth information processing systems. Silicon microring resonators (SiMRR) provide a versatile platform for all-optical switching and CMOS-compatible computing, with added advantages of high Q-factor, tunability, compactness, cascadability and scalability. A detailed theoretical analysis of ultrafast all-optical switching 2 x 2 SiMRRs has been carried out incorporating the effects of two photon absorption induced free-carrier injection and thermo optic effect. The results have been used to design …
We report on the development of an ultrafast Transmission Electron Microscope based on a laser-driven cold-field emission source. We first describe the instrument before reporting on numerical simulations of the laser-driven electron emission. These simulations predict the temporal and spectral properties of the femtosecond electron pulses generated in our ultrafast electron source. We then discuss the effects that contribute to the spatial, temporal and spectral broadening of these electron pulses during their propagation from the electron source to the sample and finally to the detectors of …
Infrared (IR) imaging has become a viable tool for visualizing various chemical bonds in a specimen. The performance, however, is limited in terms of spatial resolution and imaging speed. Here, instead of measuring the loss of the IR beam, we utilize a pulsed visible light for a high-throughput, widefield sensing of the transient photothermal effect induced by absorption of single mid-IR pulses. To extract such transient signals, we built a virtual lock-in camera synchronized to the visible probe and IR light pulses with precisely-controlled delays, allowing sub-microsecond temporal resolution…
Ultrafast Electron Microscopy (UEM) has been demonstrated to be an effective table-top technique for imaging the temporally-evolving dynamics of matter with subparticle spatial resolution on the time scale of atomic motion. However, imaging the faster motion of electron dynamics in real time has remained beyond reach. Here, we demonstrate more than an order of magnitude (16 times) enhancement in the typical temporal resolution of UEM by generating isolated 30 fs electron pulses, accelerated at 200 keV, via the optical-gating approach, with sufficient intensity for efficiently probing the elect…
Ultrafast lasers generating high repetition rate ultrashort pulses through various mode-locking methods can benefit many important applications including communication, materials processing, astronomical observation, etc. For decades, mode-locking based on dissipative four-wave-mixing (DFWM) has been fundamental in producing pulses with repetition rates on the order of gigahertz (GHz), where multiwavelength comb filters and long nonlinear components are elemental. Recently, this method has been improved using filter-driven DFWM, which exploits both the filtering and nonlinear features of silic…
Ultrafast Bessel beams demonstrate a significant capacity of structuring transparent materials with high degree of accuracy and exceptional aspect ratio. The ability to localize energy on the nanometer scale (bypassing the 100 nm milestone) makes them ideal tools for advanced laser nanoscale processing on surfaces and in the bulk. This allows to generate and combine micron and nano-sized features into hybrid structures that show novel functionalities. Their high aspect ratio and the accurate location can equally drive an efficient material modification and processing strategy on large dimensio…
We demonstrate rapid imaging based on four-wave mixing (FWM) by assessing the quality of advanced materials through measurement of their nonlinear response, exciton dephasing, and exciton lifetimes. We use a WSe$_2$ monolayer grown by chemical vapor deposition as a canonical example to demonstrate these capabilities. By comparison, we show that extracting material parameters such as FWM intensity, dephasing times, excited state lifetimes, and distribution of dark/localized states allows for a more accurate assessment of the quality of a sample than current prevalent techniques, including white…
While ultrafast laser welding is an appealing technique for bonding transparent workpieces, it is not applicable for joining silicon samples due to nonlinear propagation effects which dramatically diminishes the possible energy deposition at the interface. We demonstrate that these limitations can be circumvented by local absorption enhancement at the interface thanks to metallic nanolayer deposition. By combining the resulting exalted absorption with filament relocation during ultrafast laser irradiation, silicon samples can be efficiently joined. Shear joining strengths >4 MPa are obtained f…
Novel time-resolved imaging techniques for the investigation of ultrafast nanoscale magnetization dynamics are indispensable for further developments in light-controlled magnetism. Here, we introduce femtosecond Lorentz microscopy, achieving a spatial resolution below 100 nm and a temporal resolution of 700 fs, which gives access to the transiently excited state of the spin system on femtosecond timescales and its subsequent relaxation dynamics. We demonstrate the capabilities of this technique by spatio-temporally mapping the light-induced demagnetization of a single magnetic vortex structure…
We report on wide-field imaging of pulsatile microvascular blood flow in the exposed cerebral cortex of a mouse by holographic interferometry. We recorded interferograms of laser light backscattered by the tissue, beating against an off-axis reference beam with a 50 kHz framerate camera. Videos of local Doppler contrasts were rendered numerically by Fresnel transformation and short-time Fourier transform analysis. This approach enabled instantaneous imaging of pulsatile blood flow contrasts in superficial blood vessels over 256 x 256 pixels with a spatial resolution of 10 microns and a tempora…
Ultrafast wide-field 3D topography with extended depth of field
Key Laboratory of Light Field Manipulation and Information Acquisition, Ministry of Industry and Information Technology, School of Physical Science and Technology, Northwestern Polytechnical University（西北工业大学）
We describe a two-color pump-probe scanning magneto-optical Kerr effect (MOKE) microscope which we have developed to investigate electron spin phenomena in semiconductors at cryogenic temperatures with picosecond time and micrometer spatial resolution. The key innovation of our microscope is the usage of an ultrafast `white light' supercontinuum fiber-laser source which provides access to the whole visible and near-infrared spectral range. Our Kerr microscope allows for the independent selection of the excitation and detection energy while avoiding the necessity to synchronize the pulse trains…
We present a theoretical description of resonant radiofrequency (RF) deflecting cavities in TM$_{110}$ mode as dynamic optical elements for ultrafast electron microscopy. We first derive the optical transfer matrix of an ideal pillbox cavity and use a Courant-Snyder formalism to calculate the 6D phase space propagation of a Gaussian electron distribution through the cavity. We derive closed, analytic expressions for the increase in transverse emittance and energy spread of the electron distribution. We demonstrate that for the special case of a beam focused in the center of the cavity, the low…
We study the time-resolved reflectivity spectrum of a switched planar GaAs-AlAs microcavity. Between 5 and 40 ps after the switching (pump) pulse we observe a strong excess probe reflectivity and a change of the frequency of light trapped in the cavity up to 5 linewidths away from the cavity resonance. This frequency change does not adiabatically follow the fast-changing cavity resonance. The frequency change is attributed to an accumulated phase change due to the time-dependent refractive index. An analytical model predicts dynamics in qualitative agreement with the experiments, and points to…
Ultrashort pulsed lasers, operating through the phenomenon of mode-locking, have played a significant role in many facets of our society for 50 years, for example in the way we exchange information, measure and diagnose diseases, process materials and in many other applications. The ability to phase-lock the modes of the high-quality resonators recently exploited to demonstrate optical combs, would allow mode-locked lasers to benefit from their high optical spectral quality in order to realize novel sources such as precision optical clocks for applications to metrology, telecommunications, mic…
We report an ultrafast, parallel and beyond-the-master micro-patterning technique for ultrathin (30 nm-400 nm) non-absorbing polymer films by diffraction of a laser light through a two dimensional periodic aperture. The redistribution of laser energy absorbed by the substrate causes self-organization of polymer thin-film in the form of wrinkle like surface relief structures caused by localized melting and freezing of the thin-film. Unlike the conventional laser ablation and laser writing processes, low laser fluence is employed to only passively swell the polymer as a pre-ablative process with…
Integrating femtosecond (fs) lasers to electron microscopies has enabled direct imaging of transient structures and morphologies of materials in real time and space, namely, ultrafast electron microscopy (UEM). Here we report the development of a laser-free UEM offering the same capability of real-time imaging with high spatiotemporal resolutions but without requiring expensive fs lasers and intricate instrumental modifications. We create picosecond electron pulses for probing dynamic events by chopping a continuous beam with a radiofrequency (RF)-driven pulser, where the repetition rate of th…
We have developed a method for producing spatially stable micron-scale liquid targets of flexible shapes at kilohertz repetition rate for use in air and vacuum, by perturbing 5 and 30 μm diameter streams with femtosecond laser pulses and monitoring the temporal development of the perturbation. Using water, we have produced features such as 2.1 μm diameter droplet and 1.3 μm diameter neck with less than 0.3 μm shot-to-shot variation, with prospects for further reduction in size and variability. The use of such micron-scale targets can be expected to prevent conductive heat dissipation, enhance …
Spectroscopy of whispering-gallery mode (WGM) microresonators has become a powerful scientific tool, enabling detection of single viruses, nanoparticles, and even single molecules. Yet the demonstrated timescale of these schemes has been limited so far to milliseconds or more. Here we introduce a novel scheme that is orders of magnitude faster, capable of capturing complete spectral snapshots of WGM resonances at nanosecond timescales: cavity ring-up spectroscopy (CRUS). Based on sharply-rising detuned probe pulses, CRUS combines the sensitivity of heterodyne measurements with the highest poss…
Integrated, ultrafast all-optical polariton transistors with sub-wavelength grating microcavities
IBM Research Europe – Zurich（IBM欧洲苏黎世研究中心）；ETH Zürich（苏黎世联邦理工学院）；AMO GmbH（AMO有限公司）；RWTH Aachen University（亚琛工业大学）；Bergische Universität Wuppertal（伍珀塔尔大学）
Accelerating imaging speed in optical microscopy is often realized at the expense of image contrast, image resolution, and detection sensitivity- a common predicament for advancing high-speed and high-throughput cellular imaging. We here demonstrate a new imaging approach, called asymmetric-detection time-stretch optical microscopy (ATOM), which can deliver ultrafast label-free high-contrast flow imaging with well delineated cellular morphological resolution and in-line optical image amplification to overcome the compromised imaging sensitivity at high speed. We show that ATOM can separately r…
We propose a synthetic dimension for ultrafast free electrons based on the discrete energy sidebands in photon-induced near-field electron microscopy (PINEM). The PINEM synthetic dimension can offer a powerful way to coherently shape or modulate free-electron wavefunctions in systems such as ultrafast transmission electron microscopes, dielectric laser accelerators, and quantum free-electron lasers. As examples of this paradigm, we demonstrate Bloch oscillations, diffraction management, and linear optics effects such as Talbot self-imaging in the PINEM lattice. These effects show the potential…
We report the ultrafast laser fabrication and mid-IR characterization (3.39 microns) of four-port evanescent field directional couplers. The couplers were fabricated in a commercial gallium lanthanum sulphide glass substrate using sub-picosecond laser pulses of 1030 nm light. Straight waveguides inscribed using optimal fabrication parameters were found to exhibit propagation losses of 0.8 dB/cm. A series of couplers were inscribed with different interaction lengths, and we demonstrate power splitting ratios of between 8% and 99% for mid-IR light with a wavelength of 3.39 microns. These results…
The emission times of laser-triggered electrons from a sharp tungsten tip are directly characterized under ultrafast, near-infrared laser excitation at Keldysh parameters $6.6< γ< 19.1$. Emission delays up to 10 fs are observed, which are inferred from the energy gain of photoelectrons emitted into a synchronously driven microwave cavity. ~ fs timing resolution is achieved in a configuration capable of measuring timing shifts up to 55 ps. The technique can also be used to measure the microwave phase inside the cavity with a precision below 70 fs upon the energy resolved detection of a single e…
Mode-locked lasers, which produce ultrashort pulses in the picosecond and femtosecond range, have enabled some of the most precise measurements. However, despite significant recent progress, resolving the temporal behavior of their short pulses is still a challenge. State-of-the-art oscilloscopes with tens of picosecond resolution prevent time-resolved observations in mode-locked lasers and limit the real-time pulse evolution tracking of ultrafast lasers. Here, using the time-lens technique with a Raman amplifier, we implement an ultrafast single-shot time-microscope (TM) with a high temporal …
The use of structured ultrashort pulses with coupled spatiotemporal properties is emerging as a key tool for ultrafast manipulation. Ultrafast vector beams are opening exciting opportunities in different fields such as microscopy, time-resolved imaging, nonlinear optics, particle acceleration or attosecond science. Here, we implement a technique for the full characterization of structured time-dependent polarization light waveforms with spatiotemporal resolution, using a compact twofold spectral interferometer, based on in-line bulk interferometry and fibre-optic coupler assisted interferometr…
We have demonstrated for the first time that an array of nanoantennas (central nanotips inside sub-micron pits) on an aluminum surface, fabricated using a specific double-pulse femtosecond laser irradiation scheme, results in a 28-fold enhancement of the non-linear (three-photon) electron photoemission yield, driven by a third intense IR femtosecond laser pulse. The supporting numerical electrodynamic modeling indicates that the electron emission is increased not owing to a larger effective aluminum surface, but due to instant local electromagnetic field enhancement near the nanoantenna, contr…
This thesis centres on the development of multidimensional fluorescence imaging tools, with a particular emphasis on fluorescence lifetime imaging (FLIM) microscopy for application to biological research. The key aspects of this thesis are the development and application of tunable supercontinuum excitation sources based on supercontinuum generation in microstructured optical fibres and the development of stimulated emission depletion (STED) microscope capable of fluorescence lifetime imaging beyond the diffraction limit. The utility of FLIM for biological research is illustrated by examples o…
Nanoplasmonics has recently experienced explosive development with many novel ideas and dramatic achievements in both fundamentals and applications. The spaser has been predicted and observed experimentally as an active element -- generator of coherent local fields. Even greater progress will be achieved if the spaser could function as a ultrafast nanoamplifier -- an optical counterpart of the MOSFET (metal-oxide-semiconductor field-effect transistor). A formidable problem with this is that the spaser has the inherent feedback causing quantum generation of nanolocalized surface plasmons and sa…
Spatio-temporal shaping of electron beams is a bold frontier in electron microscopy, enabling new routes toward spatial-resolution enhancement, selective probing, low-dose imaging and faster data acquisition. Over the last decade, shaping methods evolved from passive phase plates to low-speed electrostatic and magnetostatic displays. Recently, higher shaping speed and flexibility have become feasible by the advent of ultrafast electron microscopy, embodying a swift change of paradigm that relies on using light to control free electrons. Here, we experimentally demonstrate that arbitrary transv…
Ultrafast imaging is essential in physics and chemistry to investigate the femtosecond dynamics of nonuniform samples or of phenomena with strong spatial variations. It relies on observing the phenomena induced by an ultrashort laser pump pulse using an ultrashort probe pulse at a later time. Recent years have seen the emergence of very successful ultrafast imaging techniques of single non-reproducible events with extremely high frame rate, based on wavelength or spatial frequency encoding. However, further progress in ultrafast imaging towards high spatial resolution is hampered by the lack o…
Label-free vibrational imaging by stimulated Raman scattering (SRS) provides unprecedented insight into real-time chemical distributions in living systems. Specifically, SRS in the fingerprint region can resolve multiple chemicals in a complex bio-environment using specific and well-separated Raman signatures. Yet, fingerprint SRS imaging with microsecond spectral acquisition has not been achieved due to the small fingerprint Raman cross-sections and the lack of ultrafast acquisition scheme with high spectral resolution and high fidelity. Here, we report a fingerprint spectroscopic SRS platfor…
