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TAO.

On ultrafast microscopic quantum world

Jian Wu

Published May 1, 2025• 0 citations
Publisher

Abstract

Advancements in optical quantum science and technology continuously give rise to new principles and techniques, driving the development of human civilization. Throughout the century of Nobel Prize history, several recognitions have been awarded for breakthroughs in ultrafast lasers. These achievements have played crucial roles in exploring the microscopic world and developing cutting-edge innovative technologies. While inventions like the optical microscope and X-ray diffraction have significantly enhanced our ability to uncover the nature, they mainly concentrate on obtaining steady-state information. However, the microcosm is a realm of dynamic evolution, with processes such as the vibrational motion of nuclei within molecules occurring on the picosecond (10 −12 s) or femtosecond (10 −15 s) timescales, driven fundamentally by electronic motions at the attosecond (10 −18 s) timescale. Therefore, achieving measurements and control of the evolutionary processes of the microscopic world at its characteristic time and spatial scales is indispensable for understanding physical mechanisms and achieving regulation. It will not only reveal novel physical phenomena and mechanisms but also provide new ideas for the design of new materials and structures. Utilizing ultrafast laser technology with multidimensional precise controls in the time and frequency domains, we can break through the limits of time and space measurements. Here, I will highlight our research progress in the precise measurement and control of ultrafast dynamics of molecular and macro quantum states, and provide an outlook on the frontier developments in ultrafast quantum physics.

DOI
10.1016/j.tao.2025.100009

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Advancements in optical quantum science and technology continuously give rise to new principles and techniques, driving the development of human civilization. Throughout the century of Nobel Prize history, several recognitions have been awarded for breakthroughs in ultrafast lasers. These achievements have played crucial roles in exploring the microscopic world and developing cutting-edge innovative technologies. While inventions like the optical microscope and X-ray diffraction have significantly enhanced our ability to uncover the nature, they mainly concentrate on obtaining steady-state information. However, the microcosm is a realm of dynamic evolution, with processes such as the vibrational motion of nuclei within molecules occurring on the picosecond (10 −12 s) or femtosecond (10 −15 s) timescales, driven fundamentally by electronic motions at the attosecond (10 −18 s) timescale. Therefore, achieving measurements and control of the evolutionary processes of the microscopic world at its characteristic time and spatial scales is indispensable for understanding physical mechanisms and achieving regulation. It will not only reveal novel physical phenomena and mechanisms but also provide new ideas for the design of new materials and structures. Utilizing ultrafast laser technology with multidimensional precise controls in the time and frequency domains, we can break through the limits of time and space measurements. Here, I will highlight our research progress in the precise measurement and control of ultrafast dynamics of molecular and macro quantum states, and provide an outlook on the frontier developments in ultrafast quantum physics.
The exploration of ultrafast phenomena is a frontier of condensed matter research, where the interplay of theory, computation, and experiment is unveiling new opportunities for understanding and engineering quantum materials. With the advent of advanced experimental techniques and computational tools, it has become possible to probe and manipulate nonequilibrium processes at unprecedented temporal and spatial resolutions, providing insights into the dynamical behavior of matter under extreme conditions. These capabilities have the potential to revolutionize fields ranging from optoelectronics and quantum information to catalysis and energy storage. This roadmap captures the collective progress and vision of leading researchers, addressing challenges and opportunities across key areas of ultrafast science and condensed matter. Contributions in this roadmap span the development of ab initio methods for time-resolved spectroscopy, the dynamics of driven correlated systems, the engineering of materials in optical cavities, and the adoption of FAIR principles for data sharing and analysis. Together, these efforts highlight the interdisciplinary nature of ultrafast research and its reliance on cutting-edge methodologies, including quantum electrodynamical density-functional theory, correlated electronic structure methods, nonequilibrium Green’s function approaches, quantum and ab initio simulations.
Whenever scientific tools are significantly advanced; new discoveries soon follow. My thesis work relies on advances in ultrafast laser technology that allow precise control over the shape of sub 20-fs laser pulses. This laser system enabled many new experiments that yielded significant advances in attosecond science, atomic physics; extreme nonlinear optics, quantum chemistry, coherent control, molecular physics, ultrafast optical phase modulation, EUV coherent imagines, and EUV radiation sources. By using an automated learning control algorithm coupled to our deformable mirror pulse shaper; we have demonstrated the control of a process on an attosecond time-scale for the first time. We demonstrate the manipulation of the phase of an electron wave packet, allowing us to tailor the EUV spectrum generated by high-order harmonic generation. These optimal fields were discovered by a learning algorithm that both found an unknown optimal solution; but also discovered an unknown phase-matching mechanism that occurs in the interaction of a single atom and light pulse. We control molecular vibrational and rotational coherences with the same learning algorithm; demonstrating selective control in room temperature molecules at atmospheric pressures. Moreover, we demonstrate that modifications to the algorithm can help automatically uncover the physics of the control mechanism found by the learning algorithm. We also demonstrate a new pulse-compression technique using rotational phase modulation, where optical pulses were compressed by an order of magnitude after phase modulation by a molecular rotational coherence and subsequent propagation through a transparent window. This technique will enable efficient pulse compression in the deep-UV. Finally, we measure the coherence of EUV light generated by high-harmonic upconversion of a femtosecond laser. In phase-matched hollow-fiber geometry, the EUV light exhibits the highest inherent spatial coherence of any source in this region of the spectrum. We use this source to demonstrate the coherent image with first table-top EUV radiation. Since this source exhibits full spatial coherence at very short wavelength, this light source represents has smallest inherent effective source-size of any light source yet created. We also demonstrate that the spectrum of an optical field can be determined by measuring the interference of a double-slit pattern.
Abstract The exploration of ultrafast phenomena is a frontier of condensed matter research, where the interplay of theory, computation, and experiment is unveiling new opportunities for understanding and engineering quantum materials. With the advent of advanced experimental techniques and computational tools, it has become possible to probe and manipulate nonequilibrium processes at unprecedented temporal and spatial resolutions, providing insights into the dynamical behavior of matter under extreme conditions. These capabilities have the potential to revolutionize fields ranging from optoelectronics and quantum information to catalysis and energy storage. This roadmap captures the collective progress and vision of leading researchers, addressing challenges and opportunities across key areas of ultrafast science and condensed matter. Contributions in this roadmap span the development of ab initio methods for time-resolved spectroscopy, the dynamics of driven correlated systems, the engineering of materials in optical cavities, and the adoption of FAIR principles for data sharing and analysis. Together, these efforts highlight the interdisciplinary nature of ultrafast research and its reliance on cutting-edge methodologies, including quantum electrodynamical density-functional theory, correlated electronic structure methods, nonequilibrium Green’s function approaches, quantum and ab initio simulations.
The past thirty years witnessed rapid developing of strong field physics that leads to the first generation of attosecond (10−18 s) pulses. The duration of available pulses has recently been reduced to less than 100 as, approaching the Kepler period of a classical electron revolving around the nucleus. For the first time, electron motions inside atoms, molecules and solids can be traced, probed and even steered in real time. It pushed the study on ultrafast dynamic processes into a new frontier, giving birth to attosecond physics. The development of attosecond pulses provides unprecedented coherent ultrashort XUV (extreme ultra-violet) of soft X-ray sources that enable imaging the atomic structure and resolving the related quantum dynamics for matter science. In particular, it allows the probing and monitoring of electron dynamics in the natural time scale of attoseconds with atomic spatial resolution. The generation and applications of attosecond pulses are directly related to the control and manipulation of the sub-cycle electron dynamics. Recent studies on the correlated multielectron dynamics have provided insight into the optical and dynamical properties of matter in the perspectives of time, phase and entanglement. It deepens our understanding on some of the fundamental questions, e.g., how the single or multiple photons are absorbed and how short are the quantum processes such as photoionization, tunneling ionization and charge migration. Although currently attosecond pulses are limited by the flux and pulse duration, the combination of attosecond pulses with intense infrared laser pulses paves new ways of controlling and probing electron dynamics in the domains of energy, time and space that lays the foundation for petahertz optoelectronics and attosecond pulse based transient spectroscopy. In this review, we will first briefly summarize the advancement of strong field and ultrafast physics including the relevant experimental findings, the theoretical explorations, the related technologies and the possible applications. Then we focus on the sub-cycle electron or multielectron dynamics and their manifestation on the ionization and coherent radiation properties. We start with the time behavior of Fano resonance and how it can be probed in time domain. In section 2, the correlated electron dynamics is discussed in term of anti-screening effect and Pauli effect that influence strong field ionization and high harmonic generation processes. In section 3, the coherent emission with frequency from terahertz to soft XUV and their joint measurement are discussed by emphasizing the generation mechanism of terahertz wave in two-color laser pulses. The developed high-harmonic and terahertz wave spectroscopy (HATS) is shown capable of imaging the molecular structure and dynamics. In section 4, the time-resolving of electron and hole dynamics and their coherence is proposed based on attosecond transient absorption technique. The coherence of ionization and the correlated electron dynamics is hinted crucial for electron-hole interaction. The topics are very limited and mainly selected from the perspectives of our group.
The development of quantum mechanics and quantum physics in general is one of the greatest intellectual achievements of the 20th century. Initially, quantum physicists focused on mathematically describing and understanding the laws of a micro-world, comprised of atoms, molecules and photons. Nuclei and sub-atomic particles were discovered, particle physics evolved, and complex quantum systems in chemistry and solid-state physics are now described in terms of quantum physics. Within a century, quantum physics became the framework, which allows us to describe and predict, albeit with probabilities, the behavior of the microscopic world as we know it. The powerful quantum framework led to revolutionary technical advances for a century, such as semiconductor technology and the entire electronics industry based on it, enabling computers and the information age. The development of lasers found applications in many areas of our current technologies; we use them for printers, storing and retrieving information using CDs, industrial welding, medical surgery, and for range finding and communication purposes. Medical imaging using MRI is now a routine instrument, as are precision measurements using tunneling and atomic force microscopes. Superconducting technologies are used for high magnetic fields and many more current technologies are based on and enabled by the laws of quantum physics. While the framework of quantum physics has thus proven to be extremely successful and powerful, throughout the last century there were many conceptual, and to some extent philosophical, discussions on our understanding of quantum physics. As early as the 1930s, Einstein and Schrödinger realized that quantum physics allows for some peculiar states, which Schrödinger called “entangled”, which have a non-local character and thus do find an easy interpretation in our classical world. It took a few more decades until John Bell conceived a way to quantify such states, which thus became amenable to measurements. Only in the eighties and nineties of the last century did the generation of entangled states, their characterization and their subsequent application become feasible and accessible in laboratories. Early on, Bell states were proposed for applications in quantum communication, employing protocols based on teleportation. Soon, entanglement was recognized to be useful also for sensing, for precision measurements and eventually for quantum information processing. Starting with the early concept of a trapped-ion quantum computer introduced by Ignacio Cirac and Peter Zoller in 1995, many other platforms were proposed for quantum information processing, based on superconducting quantum bits, photonic processes, engineered quantum dots and many more. The first decade of the 21st century saw an explosive development of quantum information physics, which is by now a mature field and increasingly focuses on applications. Worldwide efforts are ongoing to realize quantum networks for secure communication and to implement quantum computers. Enhanced sensing has been demonstrated using advanced quantum states, and quantum simulators have been developed, already tackling problems that are hard to compute with classical computers. While architectures for full-fledged quantum computers are already available, the realization of such computers still requires the routine implementation of error correction, which is not yet available, for full scalability. Currently, noisy intermediate-scale quantum (NISQ) processors are already used for computations and are even accessible via cloud services. Since about 2000, quantum technologies have been developed for many platforms with the aim to surpass the capablities of their classical counterparts. Many such devices now make use of entangled states, which are seen as the new resource for advanced quantum technologies. For this, describing, understanding and generally mastering the generation and manipulation of entanglement is a key element. Moreover, both hardware and software technologies have to be improved in order to better control quantum devices. Mastering quantum phenomena for communication, metrology, simulation and computation purposes is currently one of the hottest topics in science since the wide applicability of quantum technologies will revolutionize these fields. The development of advanced quantum technologies is thus seen worldwide as a strategic area for generating technical knowledge and industrial evolution. This special issue intends to showcase the breadth and impact of the ongoing research in advancing quantum technologies. We have invited a selection of renowned scientists to present their work, and we are confident that this issue will find a broad readership and attract much interest within the scientific community.
Over the past century, quantum theory has taken flight from conceptual breakthroughs, such as wave–particle duality, quantisation of energy, and the uncertainty principle, to practical tools that are the backbone of modern electronics, lasers, semiconductors, and precision measurement systems. In the twenty-first century, this progress under the regime of the second quantum revolution has acquired the ability to directly control, manipulate, and engineer individual quantum systems. Quantum technologies found their pillars in quantum properties, such as superposition, entanglement, and coherence and have exceeded the boundaries of classical physics. The steady theoretical advances, combined with experimental progress, have brought quantum concepts closer to real-life use. Significant progress has made in filed of computation, communication, sensing, navigation, medicine, cyber security, and national defense undr the guidance of quantum technology. This book chapter presents a comprehensive and pedagogical overview of quantum technologies. It highlights quantum computing, quantum communication, and quantum sensing and metrology. The shift of quantum mechanics into practical applications is discussed. Current research trends are reviewed alongside the technological and engineering challenges. The critical issues, such as decoherence, scalability, error correction, standardisation, and workforce development, are discussed, which further highlights the need for global collaboration. Both National governments and the private sector are investing heavily in quantum research. This will act as a booster for quantum technologies to revolutionise information processing, secure communications, and precision measurements. Consequently and will significantly impact the scientific and technological landscape.