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In a theoretical and experimental study published in Nature Physics, an international team of researchers demonstrates the generation of highly non-classical states of light in intense laser–atom interactions.
Advances in Laser Technology and Light-Matter Interaction
Over the past four decades, astounding advances have been made in the field of laser technologies and the understanding of light-matter interactions in the non-linear regime. Consequently, scientists have been able to carry out extremely complex experiments related to, for example, ultra-fast light pulses in the visible and infrared range. Furthermore, they have accomplished crucial milestones such as using a molecule’s own electrons to image its structure, to see how it rearranges and vibrates or breaks apart during a chemical reaction.
The development of high-power lasers allowed scientists to study the physics of ultra-intense laser-matter interactions which, in its standard version, treats ultra-strong ultra-short driving laser pulses only from a classical point of view. The famous theory coined as the “simple man’s model” or the “three-step model” – which had its 25th anniversary in 2019 – dealt with the interaction of an electron with its parent nucleus sitting in a strong laser field environment, and elegantly described it according to classical and quantum processes. However, due to the fact that these laser pulses are highly coherent and contain huge numbers of photons, the description of the interaction in the strong field has so far been incomplete, because it treated the atomic system in a quantum way but the electromagnetic field in a classical way.
Generation of Non-Classical States of Light through Intense Laser-Atom Interactions
In the current landscape, the description of the most relevant processes in ultra-intense laser-matter physics, such as high-harmonic generation, above-threshold ionization, laser-induced electron diffraction, and sequential and non-sequential multi-electron ionization, often overlooks the quantum-fluctuation effects of the laser electric field, let alone the magnetic fields. Nevertheless, the quantum nature of the entire electromagnetic field is inherently present in these processes. Consequently, a natural question arises: does this quantum nature manifest itself in observable ways? Furthermore, under what specific circumstances does this manifestation occur?
In the recent study published in Nature Physics, OPTOlogic researchers at ICFO led by ICREA Prof. Maciej Lewenstein, Max Born Institute in Berlin, in collaboration with the PhD researcher Theocharis Lamprou, led by the Research Director Paraskevas Tzallas, from FORTH, have reported on the theoretical and experimental demonstration that intense laser–atom interactions may lead to the generation of highly non-classical states of light.
Researchers obtained such results by using high-harmonic generation in atoms, where they up-convert large numbers of photons from an infrared driving laser pulse into higher-frequency photons in the extreme ultraviolet spectral range. The quantum electrodynamical theory formulated in this study predicts that a coherent initial state of the driving laser remains coherent but experiences an amplitude shift after interacting with the atomic medium.
Similarly, the harmonic modes’ quantum states become coherent with small coherent amplitudes. However, researchers can condition the driving laser pulse’s quantum state to account for this interaction, transforming it into an optical Schrödinger cat state. This state represents a quantum superposition of two distinct coherent states of light: the initial laser state and the amplitude-reduced coherent state resulting from the interaction with the atoms.
Experimental Verification and Future Implications of Non-Classical Light States
The researchers experimentally accessed the full quantum state of this laser pulse using quantum state tomography. This process requires a coherent reduction of the light’s amplitude to only a few photons on average before measuring all quantum properties of the state.
The results of this study pave the way for investigations into controlling non-classical states of ultra-intense light and exploiting conditioning approaches on physical processes relevant to high-harmonic generation. This research will hopefully create a novel and unexpected link between ultra-intense laser-matter physics, attoscience, quantum information science, and quantum technologies.
Cited article: M. Lewenstein, M. F. Ciappina, E. Pisanty, J. Rivera-Dean, P. Stammer, Th. Lamprou and P. Tzallas. Generation of optical Schrödinger “cat” states in intense laser-matter interactions, Nature Physics, 2021.
Researchers from the Physical Chemistry Department of the Fritz Haber Institute and the Max Planck Institute for the Structure and Dynamics of Matter in Hamburg have found out that ultrafast switches in material properties can be prompted by laser pulses – and why. This knowledge may enable new transistor concepts.
Advancing Transistor Technology with Light
Making the speed of electronic technology as fast as possible is a central aim of contemporary materials research. The key components of fast computing technologies are transistors: switching devices that turn electrical currents on and off very quickly as basic steps of logic operations. In order to improve our knowledge about ideal transistor materials, physicists are constantly trying to determine new methods to accomplish such extremely fast switches. Researchers from the Fritz Haber Institute of the Max Planck Society in Berlin and the Max Planck Institute for the Structure and Dynamics of Matter in Hamburg have now figured out that a novel type of ultrafast switch can be accomplished with light.
Exploring Material Property Control through Light
The physicists involved in the project, are studying how to best get materials to change their properties – to make magnetic metals non-magnetic, for example, or to change the electric conductivity of a crystal. A material’s electrical properties are strongly related to the arrangement of the electrons in the crystal. Controlling the electrons’ arrangement has been a key topic for decades. Most control methods, however, are fairly slow. “We knew that external influences like temperature or pressure variations work”, says Dr. Ralph Ernstorfer, Group Leader at the Department of Physical Chemistry at the Fritz Haber Institute and partner at the Optologic project, “but that takes time, at least a few seconds.” Those who regularly use a smartphone or computer know that a few seconds can feel like an eternity. So Dr. Ernstorfer’s group explored how to switch material properties much faster by means of light.
Ultrafast Switching with Light Pulses
Using brand new equipment at the Fritz Haber Institute, the researchers have massively cut down the switching time to only 100 femtoseconds – 0,000 000 000 000 1 of a second – by shooting ultrashort optical laser pulses at their chosen material, a semi-metallic crystal composed of tungsten and tellurium atoms. Shining light on the crystal encourages it to re-organize its internal electronic structure, which also changes the conductivity of the crystal. In addition, the scientists were able to observe exactly how its electronic structure changed. “We used a new instrument to take pictures of the transition every step of the way”, explains Dr. Samuel Beaulieu, who worked as a postdoctoral fellow with Ralph Ernstorfer at the Fritz-Haber-Institut (2018-2020) and who is now a permanent researcher at the Centre Lasers Intenses et Applications (CELIA) at CNRS-Bordeaux University.
Insight into Ultrafast Electronic Transitions
“This is amazing progress – we used to only know what the electronic structure of the material looked like after, but never during the transition,” he adds. Moreover, state-of-the-art modelling of this new process by Dr. Nicolas Tancogne-Dejean, Dr. Michael Sentef, and Prof. Dr. Angel Rubio from Max the Planck Institute for the Structure and Dynamics of Matter has revealed the origin of this novel type of ultrafast electronic transition. The laser pulse impinging on the materials changes the way electrons interact with each other, which is the driving force of this exotic transition, known as a Lifshitz transition.
Future Prospects for Ultrafast Technology
This method is bound to generate a great deal of knowledge about possible future transistor materials. The fact alone that light can drive ultrafast electronic transitions is the first step towards even quicker and more efficient technology.
Implications for Quantum Device Development
The results of this study also contribute to OPTOlogic, a project aiming to develop a new class of dissipation-less quantum devices. In this project, we aim to artificially induce and control topologically protected states using ultrafast pulses of light. We intend to move and store information with minimal energy expense, while dramatically increasing computing power. Thus, the recent achievement indicates a clear progression toward realizing this goal.
Cited article: Gierster, L., Vempati, S. & Stähler, J. Ultrafast generation and decay of a surface metal. Nat Commun 12, 978 (2021). https://doi.org/10.1038/s41467-021-21203-6
Applied Physics Reviews details the state-of-the-art of Attosecond Technology and showcases how Attosecond soft X-ray spectroscopy allows to understand the dynamics of conventional and quantum materials.
Until recently, most soft X-ray spectroscopy science and experiments were only plausible in synchrotron facilities, limiting the amount of science that could be done and augmenting the cost of these experiments. Thanks to the development of attosecond technology and the emergence of High Harmonic Generation (HHG), table-top X-ray spectroscopy technology, such as x-ray absorption near-edge spectroscopy (XANES) and extended x-ray absorption fine structure spectroscopy (EXAFS), became available and one of the most prominent tools to understand details about the structure and dynamics of composite, quantum, organic materials, as well as twisted bilayer graphene, high-temperature superconductors, and organic electronics, among many others.
In a recent paper published in Applied Physics Reviews, a team of researchers at ICFO, led by ICREA Prof. at ICFO Jens Biegert and first authored by former ICFO researcher Bárbara Buades, present a review on the field and the state-of-the-art techniques being used nowadays. The researchers further show that isolated attosecond soft x-ray pulses for x-ray absorption near edge spectroscopy (XANES) provide the element- and orbital-resolved real-time dynamics of the semi-metal TiS2.
High Harmonic Generation
HHG is an extreme form of nonlinear optics and the only technique to generate coherent short wavelength radiation. It provides pulsed radiation in the UV to SXR range and with duration of a few attoseconds, thus permitting to resolve sub-femtosecond electronic dynamics in gases, liquids and solids. In the soft x-ray range, HHG gives access to the multiple component absorption edges, which provides information about the lattice, charge and spin dynamics of a material’s components all at once. The soft x-ray regime facilitates access to the K and L-edges, related to the electronic structures of transition metal atoms and complexes.
The particular case of the Semi-metal titanium disulfide (TiS2)
Titanium disulfide is a semi-metallic material that presents extremely high electron and ion mobility, making it a very interesting material for applications such as information processing, energy harvesting or high energy density storage, e.g., efficient batteries.
Buades et al. investigated TiS2 and used attosecond soft X-ray XANES to interrogate the 3d binding orbitals of the quantum material and how their electronic properties changed upon absorbing light. Resolving with attosecond precision changes in electronic density of the Ti:3d electrons revealed a real-time view on the light-mediated flow of charge between the sulfur and titanium lattice sites.
The results of this study prove that attosecond XANES is a powerful new method to study and understand in detail the heterostructures of conventional and quantum materials. The powerful new analytical method will be a strong asset to address standing issues of our modern society such as to understand the bottlenecks in light-harvesting devices, high-density batteries, or to address energy dissipation in information storage and transmission devices.
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Image citation: Schematic illustration of how the XANES and EXAFS techniques work to observe and understand the internal orbital dynamics of materials. See figure 1 caption for a detailed description.
Researchers from Optologic publish an article in Nature communications. They demonstrate how laboratory-frame photoelectron spectra can be used directly to determine molecular structure with atomic precision through laser-induced electron diffraction (LIED). This innovative approach not only advances our understanding of molecular dynamics but also opens new avenues for precise structural analysis in various scientific fields.
Light microscopes have revolutionized our understanding of microcosmos; however, their resolution is limited to about 100 nanometers. To see how molecules bond, break, or change their structure, we need at least 1000 times better resolution.
Laser-induced electron diffraction (LIED) is a technique that allows one to pinpoint the individual atoms inside a single molecule and to see where each atom moves when the molecule undergoes a reaction. This technique proved to be an amazing tool for the imaging molecules, such as water, carbonyl sulfide or carbon disulfide. However, using a strong laser field to generate the electron diffraction presented challenges in retrieving the exact structure, since the structural resolution depended on the exact knowledge of the laser field itself.
In a study recently published in Nature Communication, ICFO researchers Aurelien Sanchez, Kasra Amini, Tobias Steinle, Xinyao Liu, led by ICREA Prof. at ICFO Jens Biegert, in collaboration with researchers from Kansas State University, Max-Planck-Institut für Kernphysik, Physikalisch-Technische Bundesanstalt, and Friedrich-Schiller-Universität Jena, have reported on an alternative and novel approach that retrieves accurate and precise information about the atomic structure without exact knowledge over the laser field. They successfully applied the method to imaging gas-phase molecule Carbonyl Sulfide (OCS), in particular on the bond lengths between the constituent atoms, showing a significant bent and asymmetrically stretched configuration of the ionized OCS+ structure.
Determining the atomic bonds of Carbonyl Sulfide
In their experiment, the scientists took a gas mixture of 1% OCS in helium and expanded it supersonically to create a molecular beam of the gas with a temperature below 90K. They then took a 3.2mm laser and exposed the molecule to the strong laser field. The interaction between the laser and the molecule produced an accelerated electron, which was released from the molecule, accelerated into the laser field and returned back to the target ion by the electric field of the laser; the re-collision of the electron with the ion structure generated a molecular imprint of the structure and, by extracting this information from the electron interference pattern and the scattering angle analysis, the scientists were capable of determining the proper structure of the molecule.
The novelty of the approach
Named ZCP-LIED, the novelty of this approach resides in the fact that the scientists came up with a very clever way to retrieve the atomic information by using the full 2D electron scattering information, mainly the energy and scattering angle spectra of the electron in the laboratory frame instead of the laser frame, which drastically improved the statistics of the results. Alongside using 2D data instead of 1D information, they also identified a distinctive feature in spectra related to what they called the zero crossing point (ZCP) positions (where the interference signal showed a null value). By carrying out the analysis over these critical points, the scientists were able to obtain from a much smaller data set more precise information on the bond lengths of the atoms that make up the molecule, reducing quite considerably the calculation time.
Validation through Quantum Chemistry Comparisons
For validation of their approach, they used various methods, compared them to quantum chemistry theoretical simulations and prove that their ZCP-LIED technique could obtain inter-nuclear distances with much higher precision, and could measure bond distances of similar length (something rather impossible to do with previous methods), that it avoided converting frames of reference, and was able to determine the molecular structure in environments where the background noise could be considerable. Taking all this into account, they reported obtaining the molecular information of 10-atom molecules, and in particular, for the carbonyl sulfide, where they saw that the molecule OCS+ had a significantly bent and asymmetrically stretched structure, different to what previous studies had determined for this molecule.
The results obtained by this study have demonstrated that the ZCP-LIED technique could be a very powerful tool to determine the molecular structure of large and more complex molecules. It could also be extended to ultrafast electron diffraction (UED) and even ultrafast X-ray diffraction (UXD) to track the geometric structure molecules in a transient phase.
Cited article: A. Sanchez, K. Amini, S.-J. Wang, T. Steinle, B. Belsa, J. Danek, A.T. Le, X. Liu, R. Moshammer, T. Pfeifer, M. Richter, J. Ullrich, S. Gräfe, C.D. Lin, J. Biegert. Molecular structure retrieval directly from laboratory-frame photoelectron spectra in laser-induced electron diffraction. Nature Communications, 10.1038/s41467-021-21855-4.
An international team of scientists reports in Nature Photonics on a novel technique for a high-brightness coherent and few-cycle duration source spanning 7 optical octaves from the UV to the THz.
Importance of Analytical Optical Methods
Analytical optical methods are crucial in modern society, facilitating rapid and secure substance identification within solids, liquids, or gases. These methods exploit the varied interaction of light with substances across the optical spectrum. For instance, the ultraviolet range accesses electronic transitions, while the terahertz detects molecular vibrations.
Application in Hyperspectral Spectroscopy
Over the years, numerous techniques have been developed to achieve hyperspectral spectroscopy and imaging, allowing scientists to observe the behavior of molecules when they fold, rotate, or vibrate. This understanding aids in the identification of cancer markers, greenhouse gases, pollutants, or harmful substances. These ultrasensitive techniques find practical application in food inspection, biochemical sensing, and even in cultural heritage preservation, facilitating the investigation of ancient object materials, paintings, or sculptures.
Challenges in Source Development
A persistent challenge has been the absence of compact sources covering a broad spectral range with sufficient brightness. While synchrotrons offer spectral coverage, they lack the temporal coherence of lasers and are typically only available in large-scale user facilities.
Recent Breakthrough in Source Development
Now, in a recent study published in Nature Photonics, an international team of researchers including OPTOlogic researchers from ICFO, the Max-Planck Institute for the Science of Light, the Kuban State University, and the Max-Born-Institute for Nonlinear Optics and Ultrafast Spectroscopy, led by ICREA Prof. at ICFO Jens Biegert, report on a compact high-brightness mid-IR-driven source combining a gas-filled anti-resonant-ring photonic crystal fiber with a novel nonlinear-crystal. The tabletop source provides a seven-octave coherent spectrum from 340 nm to 40,000 nm with spectral brightness 2-5 orders of magnitude higher than one of the brightest Synchrotron facilities.
Future Research Directions
Future research will leverage the few-cycle pulse duration of the source for the time-domain analysis of substances and materials. This will open new opportunities for multimodal measurement approaches in areas such as molecular spectroscopy, physical chemistry, and solid-state physics, among others.
Cited Article
Ugaitz Elu, Luke Maidment, Lenard Vamos, Francesco Tani, David Novoa, Michael H. Frosz, Valeriy Badikov, Dmitrii Badikov, Valentin Petrov, Philip St. J. Russell & Jens Biegert. Seven-octave high-brightness and carrier-envelope-phase-stable light source. Nature Photonics volume 15, pages277–280 (2021)
The new OPTOLogic project aims to develop a new technological platform with quantum devices and ultrashort light pulses to reduce energy loss in electronic circuits.
Since the late 1980s, energy consumption in the modern electronics industry has increased drastically. To compound the issue, electronic circuits waste, dissipate, or lose most of the energy these devices consume during the transport of charge or electricity. Knowing that our information-based society is growing at exponential rates, translating into increasing demands for consumer electronic products, studies have estimated a projected energy consumption increase of 20% by 2030. Experts expect this amount to surpass the total energy production available worldwide. This presents a major problem that demands a quick and affordable solution.
In light of this challenge, the fundamental aim of this project is to develop novel quantum materials with the express purpose of creating a new class of dissipation-less quantum devices. To achieve this, we will leverage structured ultrafast pulses of light to both induce and precisely control the topological states of these materials. In essence, topological states represent the diverse forms that matter can adopt, depending on the specific arrangement of atoms within. By manipulating these states, we anticipate a significant reduction in the major energy losses that currently plague electronic circuits.
A new class of dissipation-less devices
Researchers have proposed different solutions using conventional semiconductor materials to solve this major challenge, but none have proven effective enough. The recently launched OPTOlogic project is searching to overcome this challenge and fulfill two major goals: mitigate dissipation and save energy. Coordinated by ICREA Prof. at ICFO Jens Biegert, the consortium is comprised of ICFO, Max Plank Society (MPG), French Alternative Energies and Atomic Energy Commission (CEA), Forschungsverbund Berlin (FVB-MBI), and LightOn. This multi-disciplinary team of experts and SMEs unites world-leading experimental, theoretical, and industrial expertise in condensed matter physics, ultrafast laser technology, attoscience, quantum optics and computing, machine learning and artificial intelligence.
To achieve this, the consortium will develop a new technological platform that leverages the best aspects of topology to avoid energy loss in electronic transport. They will also incorporate light-wave-electronics to overcome limitations imposed by material properties and utilize quantum materials with quantum properties for novel information storage and processing. They will build a novel topological Qubit, the first elementary building block for the development of this innovative quantum technology, and search to perform quantum logic operations that can surpass those limitations imposed by simple binary operations.
The project will use the latest findings in ultrafast lasers, nanotechnology, and adapted quantum computing architecture to develop this new device. As ICREA Prof. at ICFO Jens Biegert remarks,
“The breakthrough of such device could result in a thousand-fold more efficient electronic circuit, with simultaneous million-to-billion-fold increase in computing clock speeds, which could move and store information with minimal energy expense, whilst achieving dramatically increased computing power”.