Latest Issue

    2023 Year 3 Volume 6 Issue

      Research Article

    • Chunmei Zhang, Graham Brown, Dong Hyuk Ko, P.B.Corkum
      2023, 3(6) DOI: 10.34133/ultrafastscience.0034
      Abstract:Recollision physics and attosecond pulse generation meld the precision of optics with collision physics. As a follow-up to our previous work, we reveal a new direction for the study of electronic structure and multielectron dynamics by exploiting the collision-physics nature of recollision. We show experimentally that, by perturbing recollision trajectories with an infrared field, photorecombination time delays can be measured entirely optically using the Cooper minimum in argon as an example. In doing so, we demonstrate the relationship between recollision trajectories and the transition moment coupling the ground and continuum states. In particular, we show that recollision trajectories are influenced by their parent ion, while it is commonly assumed they are not. Our work paves the way for the entirely optical measurement of ultrafast electron dynamics and photorecombination delays due to electronic structure, multielectron interaction, and strong-field-driven dynamics in complex molecular systems and correlated solid-state systems.  
        
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      Updated:2024-10-22
    • Ranjana Rathore, Himanshu Singhal, Vivek Dwij, Mayanak K Gupta, Abhishek Pathak, Juzer Ali Chakera, Ranjan Mittal, Aditya Prasad Roy, Arun Babu, Ruta Kulkarni, A Thamizhavel, Ayman H Said, Dipanshu Bansal
      2023, 3(6) DOI: 10.34133/ultrafastscience.0041
      Abstract:Amplitude mode is collective excitation emerging from frozen lattice distortions below the charge-density-wave (CDW) transition temperature TCDW and relates to the order parameter. Generally, the amplitude mode is non-polar (symmetry-even) and does not interact with incoming infrared photons. However, if the amplitude mode is polar (symmetry-odd), it can potentially couple with incoming photons, thus forming a coupled phonon–polariton quasiparticle that can travel with light-like speed beyond the optically excited region. Here, we present the amplitude mode dynamics far beyond the optically excited depth of ∼150 nm in the CDW phase of ∼10-μm-thick single-crystal EuTe4 using time-resolved x-ray diffraction. The observed oscillations of the CDW peak, triggered by photoexcitation, occur at the amplitude mode frequency ωAM. However, the underdamped oscillations and their propagation beyond the optically excited depth are at odds with the observation of the overdamped nature of the amplitude mode measured using meV-resolution inelastic x-ray scattering and polarized Raman scattering. The ωAM is found to decrease with increasing fluence owing to a rise in the sample temperature, which is independently confirmed using polarized Raman scattering and ab-initio molecular dynamics simulations. We rationalize the above observations by explicitly calculating two coupled quasiparticles—phonon–polariton and exciton–polariton. Our data and simulations cannot conclusively confirm or rule out the one but point toward the likely origin from propagating phonon–polariton. The observed non-local behavior of amplitude mode thus provides an opportunity to engineer material properties at a substantially faster time scale with optical pulses.  
        
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      Updated:2024-10-22
    • Surui Yang, Liang Cheng, Jingbo Qi
      2023, 3(6) DOI: 10.34133/ultrafastscience.0047
      Abstract:The study of the interaction between terahertz (THz) radiation and quantum materials has been an active area of research due to its potential for understanding fundamental physics and the development of novel technologies. In this review, we focus on the time-dependent photocurrents, behind which are the up-to-date understanding of the physical processes. We provide the recent advancements in revealing the unique properties of quantum materials via the THz emission spectroscopy. Because the theoretical interpretation of some new experimental results is still evolving, this review is intended to inspire further research in this exciting and rapidly growing field.  
        
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      Updated:2024-10-22
    • Maksim I. Paukov, Vladimir V. Starchenko, Dmitry V. Krasnikov, Gennady A. Komandin, Yuriy G. Gladush, Sergey S. Zhukov, Boris P. Gorshunov, Albert G. Nasibulin, Aleksey V. Arsenin, Valentyn S. Volkov, Maria G. Burdanova
      2023, 3(6) DOI: 10.34133/ultrafastscience.0021
      Abstract:For terahertz wave applications, tunable and rapid modulation is highly required. When studied by means of optical pump–terahertz probe spectroscopy, single-walled carbon nanotube (SWCNT) thin films demonstrated ultrafast carrier recombination lifetimes with a high relative change in the signal under optical excitation, making them promising candidates for high-speed modulators. Here, combination of SWCNT thin films and stretchable substrates facilitated studies of the SWCNT mechanical properties under strain and enabled the development of a new type of an optomechanical modulator. By applying a certain strain to the SWCNT films, the effective sheet conductance and therefore modulation depth can be fine-tuned to optimize the designed modulator. Modulators exhibited a photoconductivity change of approximately 2 times of magnitude under the strain because of the structural modification in the SWCNT network. Stretching was used to control the terahertz signal with a modulation depth of around 100% without strain and 65% at a high strain operation of 40%. The sensitivity of modulators to beam polarization is also shown, which might also come in handy for the design of a stretchable polarizer. Our results give a fundamental grounding for the design of high-sensitivity stretchable devices based on SWCNT films.  
        
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      Updated:2024-10-22
    • Tobias Flöry, Vinzenz Stummer, Justinas Pupeikis, Benjamin Willenberg, Alexander Nussbaum-Lapping, Edgar Kaksis, Franco V. A. Camargo, Martynas Barkauskas, Christopher R. Phillips, Ursula Keller, Giulio Cerullo, Audrius Pugžlys, Andrius Baltuška
      2023, 3(6) DOI: 10.34133/ultrafastscience.0027
      Abstract:Femtosecond dual-comb lasers have revolutionized linear Fourier-domain spectroscopy by offering a rapid motion-free, precise, and accurate measurement mode with easy registration of the combs beat note in the radio frequency domain. Extensions of this technique already found application for nonlinear time-resolved spectroscopy within the energy limit available from sources operating at the full oscillator repetition rate. Here, we present a technique based on time filtering of femtosecond frequency combs by pulse gating in a laser amplifier. This gives the required boost to the pulse energy and provides the flexibility to engineer pairs of arbitrarily delayed wavelength-tunable pulses for pump–probe techniques. Using a dual-channel millijoule amplifier, we demonstrate programmable generation of both extremely short, fs, and extremely long (>ns) interpulse delays. A predetermined arbitrarily chosen interpulse delay can be directly realized in each successive amplifier shot, eliminating the massive waiting time required to alter the delay setting by means of an optomechanical line or an asynchronous scan of 2 free-running oscillators. We confirm the versatility of this delay generation method by measuring χ(2) cross-correlation and χ(3) multicomponent population recovery kinetics.  
        
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      Updated:2024-10-22
    • Yudan Su, Jiaming Le, Junying Ma, Long Cheng, Yuxuan Wei, Xiaofang Zhai, Chuanshan Tian
      2023, 3(6) DOI: 10.34133/ultrafastscience.0042
      Abstract:The surface/interface species in perovskite oxides play essential roles in many novel emergent physical phenomena and chemical processes. With low eigen-energies in the terahertz region, such species at buried interfaces remain poorly understood due to the lack of feasible surface-specific spectroscopic probes to resolve the resonances. Here, we show that polarized phonons and two-dimensional electron gas at the interface can be characterized using surface-specific nonlinear optical spectroscopy in the terahertz range. This technique uses intra-pulse difference frequency mixing process, which is allowed only at the surface/interface of a centrosymmetric medium. Submonolayer sensitivity can be achieved using the state-of-the-art detection scheme for the terahertz emission from the surface/interface. Through symmetry analysis and proper polarization selection, background-free Drude-like nonlinear response from the two-dimensional electron gas emerging at the LaAlO3/SrTiO3 or Al2O3/SrTiO3 interface was successfully observed. The surface/interface potential, which is a key parameter for SrTiO3-based interface superconductivity and photocatalysis, can now be determined optically in a nonvacuum environment via quantitative analysis on the phonon spectrum that was polarized by the surface field in the interfacial region. The interfacial species with resonant frequencies in the THz region revealed by our method provide more insights into the understanding of physical properties of complex oxides.  
        
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      Updated:2024-10-22
    • Yudong Chen, Zongyuan Fu, Baochang Li, Sainan Peng, Bingbing Zhu, Guangyu Fan, Yi Liu, Chengyuan Ding, Cheng Jin, Zhensheng Tao
      2023, 3(6) DOI: 10.34133/ultrafastscience.0045
      Abstract:Nonadiabatic phase matching of high-harmonic generation (HHG) driven by few-cycle laser pulses is essential for extending harmonic energy and generating isolated attosecond pulses. However, understanding nonadiabatic HHG is challenging due to the complex interplay of various optical phases driven by temporally and spatially varying laser fields. Theoretical calculations typically rely on computationally demanding 3-dimensional simulations, which can make it difficult to extract the essential features of nonadiabatic HHG. In this work, we develop a computationally efficient 2-dimensional model that directly considers various phase contributions of HHG. Our model can well explain the experimentally observed pressure and intensity-dependent behaviors of different harmonic orders. By appropriately parameterizing the single-atom response, our model can also estimate the variation of HHG spectra under different driving conditions. Our model can provide an efficient tool for the design and optimization of HHG-based applications.  
        
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      Updated:2024-10-22

      Review Article

    • Tomoyoshi Inoue, Takashi Kakue, Kenzo Nishio, Toshihiro Kubota, Osamu Matoba, Yasuhiro Awatsuji
      2023, 3(6) DOI: 10.34133/ultrafastscience.0043
      Abstract:In the last few decades, there have been several advances in ultrafast imaging of light propagation with light-in-flight recording by holography (LIF holography), which can capture light propagation as a motion picture with a single shot in principle. Here, we review the recent advances in LIF holography by considering the perspectives of various development of functional imaging techniques and evaluation of LIF holography with numerical simulation methods. The methods for recording multiple motion pictures such as a space-division multiplexing, a pixel-by-pixel-based space-division multiplexing, and an angular multiplexing technique are added extend the capability of LIF holography. The numerical simulation models used for investigating the image characteristics of LIF hologram are discussed. Finally, a summary and conclusion of recent advances in LIF holography is presented.  
        
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      Updated:2024-10-22
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