Advances in high-order harmonic generation sources for time-resolved investigations
Maurizio Reduzzi, Paolo Carpeggiani, Sergei Kühn, Francesca Calegari, Mauro Nisoli, Salvatore Stagira, Caterina Vozzi, Peter Dombi, Subhendu Kahaly, Paris Tzall… 展开作者
Maurizio Reduzzi, Paolo Carpeggiani, Sergei Kühn, Francesca Calegari, Mauro Nisoli, Salvatore Stagira, Caterina Vozzi, Peter Dombi, Subhendu Kahaly, Paris Tzallas, Katalin Varju, Karoly Osvay, Giuseppe Sansone
We review the main research directions ongoing in the development of high-harmonic generation-based extreme ultraviolet sources for the synthesization and application of trains and isolated attosecond pulses to time-resolved spectroscopy. A few experimental and theoretical works will be discussed in connection to well-established attosecond techniques. In this context, we present the unique possibilities offered for time-resolved investigations on the attosecond timescale by the new Extreme Light Infrastructure Attosecond Light Pulse Source, which is currently under construction.
We extend image scanning microscopy to second harmonic generation (SHG) by extracting the complex field amplitude of the second-harmonic beam. While the theory behind coherent image scanning microscopy (ISM) is known, an experimental demonstration wasn't yet established. The main reason is that the naive intensity-reassignment procedure cannot be used for coherent scattering as the point spread function is now defined for the field amplitude rather than for the intensity. We use an inline interferometer to demonstrate super-resolved phase-sensitive SHG microscopy by applying the ISM reassignme…
We study the crystal-momentum-resolved contributions to the high-order harmonic generation (HHG) in band-gap materials, and identify the relevant initial crystal momenta for the first and higher plateaus of the HHG spectra. We do so by using a time-dependent density-functional theory model of one-dimensional linear chains. We introduce a self-consistent periodic treatment for the infinitely extended limit of the linear chain model, which provides a convenient way to simulate and discuss the HHG from a perfect crystal beyond the single-active-electron approximation. The multi-plateau spectral f…
Space-time resolved simulation of femtosecond nonlinear light-matter interactions using a holistic quantum atomic model: Application to near-threshold harmonics
Recent progress in laser-based high-repetition rate extreme ultraviolet (EUV) lightsources and multidimensional photoelectron spectroscopy enable the build-up of a new generation of time-resolved photoemission experiments. Here, we present a setup for time-resolved momentum microscopy driven by a 1 MHz femtosecond EUV table-top light source optimized for the generation of 26.5 eV photons. The setup provides simultaneous access to the temporal evolution of the photoelectron's kinetic energy and in-plane momentum. We discuss opportunities and limitations of our new experiment based on a series o…
Attosecond metrology sensitive to sub-optical-cycle electronic and structural dynamics is opening up new avenues for ultrafast spectroscopy of condensed matter. Using intense lightwaves to precisely control the extremely fast carrier dynamics in crystals holds great promise for next-generation electronics and devices operating at petahertz bandwidth. The carrier dynamics can produce high-order harmonics of the driving light field extending up into the extreme-ultraviolet region. Here, we introduce polarization-state-resolved high-harmonic spectroscopy of solids, which provides deeper insights …
We present an experimental study on the photoionization dynamics of non-resonant one-color two-photon single valence ionization of neutral argon atoms. Using 9.3 eV photons produced via high harmonic generation and a 3-D momentum imaging spectrometer, we detect the photoelectrons and ions produced from non-resonant two-photon ionization in coincidence. Photoionization from the $3p$ orbital produces a photoelectron scattering wave function with $p$ and $f$ partial wave components, which interfere and result in a photoelectron angular distribution with peak amplitude perpendicular to the VUV pol…
We demonstrate a novel algorithmic approach for the second-harmonic-generation (SHG) frequency-resolved optical gating (FROG) ultrashort-pulse-measurement technique that always converges and, for complex pulses, is also much faster. It takes advantage of the Paley-Wiener Theorem to retrieve the precise pulse spectrum (half the desired information) directly from the measured trace. It also uses a multi-grid approach, permitting the algorithm to operate on smaller arrays for early iterations and on the complete array for only the final few iterations. We tested this approach on more than 25,000 …
Wavefront sensors are an important tool to characterize coherent beams of extreme ultraviolet radiation. However, conventional Hartmann-type sensors do not allow for independent wavefront characterization of different spectral components that may be present in a beam, which limits their applicability for intrinsically broadband high-harmonic generation (HHG) sources. Here we introduce a wavefront sensor that measures the wavefronts of all the harmonics in a HHG beam in a single camera exposure. By replacing the mask apertures with transmission gratings at different orientations, we simultaneou…
Strong field driven electric currents in condensed matter systems open new frontiers in petahertz electronics. In this regime new challenges arise as the role of the band structure and the quantum nature of electron-hole dynamics have yet to be resolved. Here we reveal the underlying attosecond dynamics that dictates the temporal evolution of carriers in multi-band solid state systems, via high harmonic generation (HHG) spectroscopy. We demonstrate that when the electron-hole relative velocity approaches zero, enhanced quantum interference leads to the appearance of spectral caustics in the HH…
High harmonic generation in solids provides us compact and coherent UV sources. Our simulations illustrate abnormal harmonic yield dependence on the intensity of driving or pre-excitation pulses. A multielectron interference model is proposed to reveal the mechanism of the extreme nonlinear optical phenomena. We find that the $k$-resolved intraband harmonic demonstrates different symmetry, phase, and amplitude, which can be observed by using a resonant pre-excitation pulse. The position of the interference minimum obtained by solving the semiconductor Bloch equations agrees well with that obta…
We present a table-top extreme ultraviolet (XUV) beamline for measuring time- and frequency-resolved XUV excited optical luminescence (XEOL) with additional femtosecond-resolution XUV transient absorption spectroscopy functionality. XUV pulses are generated via high-harmonic generation using a near-infrared pulse in a noble gas medium, and focused to excite luminescence from a solid sample. The luminescence is collimated and guided into a streak camera, where its spectral components are temporally resolved with picosecond temporal resolution. We time-resolve XUV excited luminescence and compar…
We demonstrate an all-optical approach for precise characterization of attosecond extreme ultraviolet pulses. Isolated attosecond pulse is produced from high order harmonics using intense driving pulse with proper gating technique. When a weak field is synchronized with the driver, it perturbs the harmonics generation process via altering the accumulated phase of the electron trajectories. The perturbed harmonic spectrum can be formulated as a convolution of the unperturbed dipole and a phase gate, implying the validity of complete reconstruction of isolated attosecond pulses using conventiona…
With its direct correspondence to electronic structure, angle-resolved photoemission spectroscopy (ARPES) is a ubiquitous tool for the study of solids. When extended to the temporal domain, time-resolved (TR)-ARPES offers the potential to move beyond equilibrium properties, exploring both the unoccupied electronic structure as well as its dynamical response under ultrafast perturbation. Historically, ultrafast extreme ultraviolet (XUV) sources employing high-order harmonic generation (HHG) have required compromises that make it challenging to achieve a high energy resolution - which is highly …
We propose and numerically demonstrate a new very robust and highly selective method for femtosecond time-resolved chiral spectroscopy using high harmonic generation (HHG). The method is based on dynamical symmetry breaking from chiral media, and relies only on intense electric-dipole transitions, and not on the interplay of electric and magnetic dipoles. The symmetry breaking results in the emission of a strong chiral signal in the form of otherwise 'forbidden' harmonics (i.e., that are not emitted from achiral media). The intensity of these symmetry-forbidden harmonics is directly correlated…
Characterizing and controlling electronic properties of quantum materials require direct measurements of non-equilibrium electronic band structures over large regions of momentum space. Here, we demonstrate an experimental apparatus for time- and angle-resolved photoemission spectroscopy using high-order harmonic probe pulses generated by a robust, moderately high power (20 W) Yb:KGW amplifier with tunable repetition rate between 50 and 150 kHz. By driving high-order harmonic generation (HHG) with the second harmonic of the fundamental 1025 nm laser pulses, we show that single-harmonic probe p…
Second Harmonic Generation Microscopy (SHG) is generally acknowledged as a powerful tool for the label-free 3D visualization of tissues and advanced materials, with one of its most popular applications being collagen imaging. Although the great need, progress in super-resolved SHG imaging lags behind the developments reported over the past years in fluorescence-based optical nanoscopy. In this work, we quantitatively show on collagenous tissues that by combining SHG imaging with re-scan microscopy resolutions that surpass the diffraction limit with ~1.4x become available. Besides Re-scan Secon…
Atomic excitation to excited states in strong laser field is the key to high-order harmonic generation below ionization threshold, yet remains unclear mainly due to the lack of proper detection methods. We propose a frequency-resolved photon-electron spectroscopy technique to reconstruct population of excited states with the second delayed laser pulse. The technique utilizes Fourier transformation to separate ionization from different excited states to different positions on the spectrum. With the advantage of separation, we provide a scheme to reconstruct populations on different excited stat…
Collinear double-pulse seeding of the High-Gain Harmonic Generation (HGHG) process in a free-electron laser (FEL) is a promising approach to facilitate various coherent nonlinear spectroscopy schemes in the extreme ultraviolet (XUV) spectral range. However, in collinear arrangements using a single nonlinear medium, temporally overlapping seed pulses may introduce nonlinear mixing signals that compromise the experiment at short time delays. Here, we investigate these effects in detail by extending the analysis described in a recent publication (Wituschek et al., Nat. Commun., 11, 883, 2020). Hi…
Direct imaging of molecular dynamics is a long-standing goal in physics and chemistry. As an emerging tool, high-harmonic spectroscopy (HHS) enables accessing molecular dynamics on femtosecond to attosecond time scales. However, decoding information from the harmonic signals is usually painstaking due to the coherent nature of high-harmonic generation (HHG). Here we show that this obstacle can be effectively overcome by exploiting machine learning in HHS. Combining the machine learning with an angle-resolved HHS method, we demonstrate that the rich dynamics of molecular rotational wave packet …
High-order harmonic generation by femtosecond laser pulse in the presence of a moderately strong terahertz (THz) field is studied under the strong field approximation, showing a simple proportionality of near-cutoff even-order harmonic (NCEH) amplitude to the THz electric field. The formation of the THz induced-NCEHs is analytically shown for both continuous wave and Gaussian pulse. The perturbation analysis with regard to the frequency ratio of the THz field to the femtosecond pulse shows the THz-induced NCEHs originates from its first-order correction, and the available parametric conditions…
Quantum Trajectory Separation and Attosecond Mapping in Liquid High-Harmonic Generation
Wuhan National Laboratory for Optoelectronics and School of Physics, Huazhong University of Science and Technology（华中科技大学光电国家实验室和物理学院）；School of Mathematics and Physics, China University of Geosciences（中国地质大学数学与物理学院）；Hubei Key Laboratory of Optical Information and Pattern Recognition, Wuhan Institute of Technology（武汉工程大学湖北省光学信息与模式识别重点实验室）
We investigate the electron quantum path interference effects during high harmonic generation in atomic gas medium driven by ultrashort chirped laser pulses. To achieve that, we identify and vary the different experimentally relevant control parameters of such a driving laser pulse influencing the high harmonic spectra. Specifically, the impact of the pulse duration, peak intensity and instantaneous frequency is studied in a self-consistent manner based on Lewenstein formalism. Simulations involving macroscopic propagation effects are also considered. The study aims to reveal the microscopic b…
We study the time-resolved fluorescence spectrum in two-level systems interacting with an incident coherent field, both in the weak and intermediate coupling regimes. For a single two-level system in the intermediate coupling case, as time flows, the spectrum develops distinct features, that are not captured by a semi-classical treatment of the incident field. Specifically, for a field on resonance with the atomic transition energy, the usual Mollow spectrum is replaced by a four peak structure, and for a frequency that is half of the atomic transition energy, the time-dependent spectrum devel…
We establish time-resolved high harmonic generation (tr-HHG) as a powerful spectroscopy for photoinduced dynamics in strongly correlated materials through a detailed investigation of the insulator-to-metal transitions in vanadium dioxide. We benchmark our technique by comparing our measurements to established momentum-resolved ultrafast electron diffraction, and theoretical density functional calculations. Tr-HHG allows distinguishing of individual dynamic channels, including a transition to a thermodynamically hidden phase. In addition, the HHG yield is shown to be modulated at a frequency ch…
Time- and angle-resolved photoelectron spectroscopy (trARPES) employing a 500 kHz extreme-ultravioled (XUV) light source operating at 21.7 eV probe photon energy is reported. Based on a high-power ytterbium laser, optical parametric chirped pulse amplification (OPCPA), and ultraviolet-driven high-harmonic generation, the light source produces an isolated high-harmonic with 110 meV bandwidth and a flux of more than $10^{11}$ photons/second on the sample. Combined with a state-of-the-art ARPES chamber, this table-top experiment allows high-repetition rate pump-probe experiments of electron dynam…
Optically Active Fractional Wannier-Center Displacement Drives Giant Second-Harmonic Generation
University of Science and Technology of China（中国科学技术大学）；Hefei Comprehensive National Science Center（合肥综合性国家科学中心）；Hefei National Laboratory, University of Science and Technology of China（中国科学技术大学合肥国家实验室）
It is of fundamental importance but challenging to simultaneously identify atomic and magnetic configurations of two-dimensional van der Waals materials. In this work, we show that the nonreciprocal second-harmonic generation (SHG) can be a powerful tool to answer this challenge. Despite the preserved lattice inversion symmetry, the interlayer antiferromagnetic order and spin-orbit coupling generate enhanced SHG in PT-symmetric bilayer chromium triiodide (CrI3). Importantly, the in-plane polarization-resolved SHG is sensitive to subtly different interlayer structures that cannot be told by lin…
The long standing issue of separating resonant from non-resonant processes in extreme nonlinear optics is resolved. The theoretical formalism is applied to high harmonic generation (HHG) in solids and reveals a deeper view into the dominant laser and material dependent mechanisms. Mid-infrared driven HHG in semiconductors is dominated by the resonant interband current. As a result of the dynamic Stark shift, virtual processes gain in importance in near-infrared driven HHG in dielectrics. Finally, our analysis identifies limitations of microscopic one-electron-hole theories.
The quest for mapping the femtosecond dynamics of the electronic band structure of complex materials via Time- and Angle-Resolved Photoelectron Spectroscopy (TR-ARPES) over their full First Brillouin Zone is pushing the development of schemes to efficiently generate ultrashort photon pulses in the VUV-range of photon energies. At present, the critical aspect is to combine a high photon energy with high photoemission count rates and a small pulse-bandwidth, necessary to achieve high energy resolution in ARPES, while preserving a good time resolution and mitigating space-charge effects. Here we …
We demonstrate the simultaneous generation of second, third, and fourth harmonic from a single dielectric Bismuth Ferrite nanoparticle excited by a telecom fiber laser at 1560 nm. We first characterize the signals associated with different nonlinear orders in terms of spectrum, excitation intensity dependence, and relative signal strengths. Successively, on the basis of the polarization-resolved emission curves of the three harmonics, we discuss the interplay of susceptibility tensor components at the different orders and we show how polarization can be used as an optical handle to control the…
Tunable coherent light sources operating in the vacuum ultraviolet (VUV) region in 100-200-nm (6-12 eV) wavelength range have important spectroscopic applications in many research fields, including time-resolved angle-resolved photoemission spectroscopy (ARPES). Recent advances in laser technology have enabled the upconversion of visible femtosecond lasers to the vacuum and extreme ultraviolet regions. However, the complexity of their experimental setups and the scarcity of bulk nonlinear crystals for VUV generation have hampered its widespread use. Here, we propose the use of a free-standing …
The present work discusses the impact of vacancy defects in solid high-order harmonic generation. The total energy cutoff of the high-order harmonic spectrum increases as a function of concentration of vacancy defects, and the total spectrum gradually turns into a single slanted spectrum without having an abrupt transition between primary and secondary plateaus. The spectral intensity of the below-band-gap harmonics in a solid with vacancy defects is enhanced significantly in comparison to the harmonics in a pristine solid. The changes in the harmonic spectra are understood in terms of their e…
Nonadiabatic dynamics around an avoid crossing or a conical intersection play a crucial role in the photoinduced processes of most polyatomic molecules. The present work shows that the topological phase in conical intersection makes the behavior of pump-probe high-order harmonic spectroscopy different from the case of avoid crossing. The coherence built up when the system crosses the avoid crossing will lead to the oscillatory behavior of the spectrum, while the geometric phase erodes these oscillations in the case of conical intersection. Additionally, the dynamical blueshift and the splittin…
Angle-resolved second harmonic generation (SHG) spectra of ZnO microwires show characteristic Fano resonances in the spectral vicinity of exciton-polariton modes. The output SHG spectra after SHG interacting with exciton polariton shows a resonant enhancement peak accompanied by a suppression dip originating from the constructive and destructive interference respectively. It is demonstrated that the Fano line shape, and thus the Fano asymmetry parameter q, can be tuned by the phase-shift of the two channels. The phase-dependent q was calculated and the model describes our experimental results …
Angle-resolved photoemission spectroscopy with 9-eV photon-energy pulses generated in a gas-filled hollow-core photonic crystal fiber
本文利用充气空芯光子晶体光纤中光孤子的传输特性，研究了一种新的紫外辐射源，并将其应用于角分辨光电子能谱（ARPES）。只有几μJ能量的近红外飞秒脉冲在充气光纤内产生5.5至9 eV的真空紫外（VUV）辐射。这些脉冲被用来测量的拓扑绝缘体Bi 2 Se 3的能带结构的信噪比与高次谐波从气体射流获得。两个数量级的效率增益承诺在数百kHz甚至MHz的重复率下进行时间分辨的ARPES测量，光子能量覆盖大多数材料的第一布里渊区。
Vacuum ultraviolet (VUV) light is critical for the study of molecules and materials, but the generation of femtosecond pulses in the VUV region at high repetition rates has proven difficult. Here, we demonstrate the efficient generation of VUV light at MHz repetition rates using highly cascaded four-wave mixing processes in a negative-curvature hollow-core fiber. Both even and odd order harmonics are generated up to the 15th harmonic (69 nm, 18.0 eV), with high energy resolution of ~40 meV. In contrast to direct high harmonic generation, this highly cascaded harmonic generation process require…
