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Deep within every piece of magnetic material, electrons dance to the invisible tune of quantum mechanics. Their spins, akin to tiny atomic tops, dictate the magnetic behavior of the material they inhabit. This microscopic ballet is the cornerstone of magnetic phenomena, and it's these spins that a team of JILA researchers—headed by JILA Fellows and University of Colorado Boulder physics professors Margaret Murnane and Henry Kapteyn—has learned to control with remarkable precision, potentially redefining the future of electronics and data storage. 

As reported in a new Science Advances paper, the JILA team and collaborators from universities in Sweden, Greece, and Germany probed the spin dynamics within a special material known as a Heusler compound: a mixture of metals that behaves like a single magnetic material. For this study, the researchers utilized a compound of cobalt, manganese, and gallium, which behaved as a conductor for electrons whose spins were aligned upwards and as an insulator for electrons whose spins were aligned downwards.

Using a form of light called extreme ultraviolet high-harmonic generation (EUV HHG) as a probe, the researchers could track the re-orientations of the spins inside the compound after exciting it with a femtosecond laser, which caused the sample to change its magnetic properties. The key to accurately interpreting the spin re-orientations was the ability to tune the color of the EUV HHG probe light.
“In the past, people haven't done this color tuning of HHG,” explained co-first author and JILA graduate student Sinéad Ryan. “Usually, scientists only measured the signal at a few different colors, maybe one or two per magnetic element at most.” In a historic first, the JILA team tuned their EUV HHG light probe across the magnetic resonances of each element within the compound to track the spin changes with a precision down to femtoseconds (a quadrillionth of a second).

“On top of that, we also changed the laser excitation fluence, so we were changing how much power we used to manipulate the spins,” Ryan elaborated, highlighting that that step was also an experimental first for this type of research. By changing the power, the researchers could influence the spin changes within the compound.

To study nanoscale patterns in tiny electronic or photonic components, a new method based on lensless imaging allows for near-perfect high-resolution microscopy. This is especially important at wavelengths shorter than ultraviolet, which can image with higher spatial resolution than visible light but where image-forming optics are imperfect. 

The most powerful form of lensless imaging is called ptychography, which works by scanning a laser-like beam across a sample, collecting the scattered light, and then using a computer algorithm to reconstruct an image of the sample. 

While ptychography can visualize many nanostructures, this special microscope has trouble analyzing samples with very regular, repeating patterns. This is because the scattered light does not change as a periodic sample is scanned, so the computer algorithm gets confused and cannot reconstruct a good image.

Taking on this challenge, recently graduated Ph.D. researchers Bin Wang and Nathan Brooks, working with JILA Fellows Margaret Murnane and Henry Kapteyn, developed a novel method that uses short-wavelength light with a special vortex or donut shape to scan these repeating surfaces, resulting in more varied diffraction patterns. This allowed the researchers to capture high-fidelity image reconstructions using this new approach, which they recently published in Optica. This result will also be highlighted in the Optica Magazine Optics and Photonics News in the annual highlights of Optics in 2023. 

To engineer materials with unique properties, like superconductivity, scientists dive into the quantum interactions between electrons and vibrational particles called phonons. When electrons and phonons strongly interact, they behave as “quasi” particles, not single isolated particles. These interactions occur on extremely short timescales: electrons interact with each other in femtoseconds (10^-15 seconds) or even faster, while phonons respond more slowly, within hundreds of femtoseconds, since the heavier atoms move more slowly than electrons. 

To investigate these interactions, scientists often change a material's temperature, pressure, or chemical composition and measure its electrical properties to learn about the interactions. However, materials that host different interactions can exhibit very similar properties, making it challenging to pinpoint the exact nature of these interactions.

To overcome this issue, JILA graduate student Yingchao Zhang, working with JILA Fellows Henry Kapteyn and Margaret Murnane and University of Colorado Boulder physics professor Rahul Nandkishore, utilized a powerful new method to precisely identify phonon interactions within quantum materials, the results of which were published in Nano Letters. Using ultraprecise, timed laser pulses, and extreme ultraviolet pulses, they measured the response times and saw precisely how the electrons and phonons interacted.  This method paves the way for better control and manipulation of quantum materials.

Quantum materials, a fascinating class of materials that harness the power of quantum mechanics, are revolutionizing modern science and technology. Quantum materials often possess exotic states of matter, such as superconductivity or magnetic ordering, that defy conventional understanding and can be manipulated for various technological applications. To further enhance and manipulate the intriguing characteristics of quantum materials, researchers leverage nanostructuring—the ability to precisely control the geometry on the atomic scale. Specifically, nanostructuring provides the ability to manipulate and fine-tune the electrical and thermal properties of quantum and other materials. This can result, for example, in designer structures that conduct current very well, but impede heat transport. A related critical challenge for a broad range of nanotechnologies is the need for more efficient cooling so that the nanodevices do not overheat during operation. To better understand heat transport at the nanoscale, JILA Fellows Margaret Murnane, Henry Kapteyn, and their research groups within the STROBE NSF Center, JILA, and the University of Colorado Boulder, created the first general analytical theory of nanoscale-confined heat transport, that can be used to engineer heat transport in 3D nanosystems—such as nanowires and nanomeshes—that are of great interest for next-generation energy-efficient devices. This discovery was published in NanoLetters. 

Though microscopes have been in use for centuries, there is still much that we cannot see at the smallest length scales. Current microscopies range from the simple optical microscopes used in high school science classes, to x-ray microscopes that can image through visibly-opaque objects, to electron microscopes that use electrons instead of light to capture images of vaccines and viruses. However, there is a great need to see beyond the static structure of an object—to be able capture a nano- or biosystem functioning in real time, or to visualize the magnetic field on nanometer scales. A team of researchers from the STROBE Center have been working together to overcome these challenges. STROBE is an NSF Science and Technology Center led by JILA Fellow Margaret Murnane. The large and multidisciplinary collaboration included Chen-Ting Liao and the Kapteyn-Murnane group from JILA, the Miao and Osher groups from University of California Los Angeles, Ezio Iacocca from University of Colorado, Colorado Springs, David Shapiro and collaborators at Lawrence Berkley National Laboratory, and the Badding and Crespi groups from Pennsylvania State University. They developed and implemented a new method to use x-ray beams to capture the 3D magnetic texture in a material with very high 10-nanometer spatial resolution for the first time. They published their new technique and new scientific findings in Nature Nanotechnology.

Lasers have not only fascinated scientists for decades, but they have also become an integral part of many electronic devices. To create scientific-grade lasers, physicists try to control the temporal, spatial, phase, and polarization properties of the laser beam’s pulse to be able to manipulate it. One of these properties is called the orbital angular momentum (OAM), and its phase, or shape, swirls as the doughnut-shaped laser beam travels through space. There are two types of OAM, spatial (S-OAM) and spatial-temporal (ST-OAM). S-OAM describes the angular momentum of the laser beam that is parallel to the light source's propagation direction. In contrast, ST-OAM has angular momentum that moves in a motion perpendicular to the light source’s  propagation direction, which creates a time component to the momentum  [1, 2].  Because of these differences, ST-OAM is more difficult to study due to this time component. According to senior scientist Dr. Chen-Ting Liao: “The problem is that ST-OAM is very difficult to see or measure. And if we can't see or measure this easily, there's no way we can fully understand and optimize it, let alone use it for potential future applications.” To try to overcome this difficulty, a collaboration led by Dr. Liao and other researchers, including JILA Fellows Margaret Murnane and Henry Kapteyn, worked out a method to image and better analyze ST-OAM beams. Their work was subsequently published in ACS Photonics and featured on the cover [3].

More than 400 years later, scientists are in the midst of an equally-important revolution. They’re diving into a previously-hidden realm—far wilder than anything van Leeuwenhoek, known as the “father of microbiology,” could have imagined. Some researchers, like physicists Margaret Murnane and Henry Kapteyn, are exploring this world of even tinier things with microscopes that are many times more precise than the Dutch scientist’s. Others, like Jun Ye, are using lasers to cool clouds of atoms to just a millionth of a degree above absolute zero with the goal of collecting better measurements of natural phenomena. 

Physicists develop some of the most cutting-edge technologies, including new types of lasers, microscopes, and telescopes. Using lasers, physicists can learn more about quantum interactions in materials and molecules by taking snapshots of the fastest processes, and many other things. While lasers have been used for decades, their applications in technology continue to evolve. One such application is to generate and control x-ray laser light sources, which produce much shorter wavelengths than visible light. This is important because progress in developing x-ray lasers with practical applications had essentially stalled for over 50 years. Fortunately, researchers are beginning to change this by using new approaches. In a paper published in Science Advances, a JILA team, including JILA Fellows Margaret Murnane, and Henry Kapteyn, manipulated laser beam shapes to better control properties of x-ray light.

Last week, U.S. Rep. Joe Neguse got a first-hand look at the future of ultrafast lasers, record-setting clocks, and quantum computers on the CU Boulder campus. Neguse visited the university Thursday to tour facilities at JILA, a research partnership between CU Boulder and the National Institute of Standards and Technology (NIST).

The second quantum revolution is underway, a period marked by significant advances in quantum technology, and huge discoveries within quantum science. From tech giants like Google and IBM, who build their own quantum computers, to quantum network startups like Aliro Quantum, companies are eager to profit from this revolution. However, doing so takes a new type of workforce, one trained in quantum physics and quantum technology. The skillset required for this occupation is unique, and few universities expose students to real-world quantum technology. 

Two new papers from the Murnane and Kapteyn group are changing the way heat transport is viewed on a nanoscale, and explain the group’s surprising finding that nanoscale heat transport can be far more efficient than originally thought. One of these papers, published in the Proceedings of the National Academy of Sciences (PNAS), explains heat transport for the tiniest of hotspots, with sizes <100 nm. The other, published in American Chemical Society Nano (ACS Nano), presents a theory that is applicable to larger arrays of hotspots. Both papers postulate theories that can fully explain the surprising data collected by the team of researchers, showing that heat transport on scale lengths relevant to a wide range of nanotechnologies is more efficient than originally thought.

For laser science, one major goal is to achieve full control over the spatial, temporal and polarization properties of light, and to learn how to precisely manipulate these properties.  A  property of light is called the Orbital Angular Momentum (OAM), that depends on the spatial distribution of the phase (or crests) of a doughnut-shaped light beam. More recently, a new variant of OAM was discovered - called the spatial-temporal OAM (ST-OAM), with much more elusive properties, since the phase/crests of light evolve both temporally and spatially. In a collaboration led by senior scientist Dr. Chen-Ting Liao, working with graduate student Guan Gui and Nathan Brooks and JILA Fellows Margaret Murnane and Henry Kapteyn, the team explored how such beams change after propagating through nonlinear crystals that can change their color. The team published theri results in Nature Photonics. 

Electronics keep shrinking. As they shrink the properties of the materials that make them change too. 

In a new study from the Kapteyn-Murnane Group, ultrafast laser pulses can precisely cut through and manipulate the interaction between electrons and phonons in tantalum diselenide, changing its properties.

Researchers at JILA and the University of Salamanca have found a new property of light, one that creates a whirling vortex that can speed itself up. 

By using ultrafast lasers to measure the temperature of electrons, JILA researchers have discovered a never-before-seen state in an otherwise standard semiconductor. This research is the most recent demonstration of a new technique, called ultrafast electron calorimetry, which uses light to manipulate well-known materials in new ways.

The hardest problems are never solved by one person. They are solved by teams; or in the case of science, collaborations. It took a collaboration of 17 researchers, including four JILA fellows and another six JILA affiliates, just a little over five years to achieve robust polarization control over isolated attosecond (one billionth of a billionth of a second) pulses of extreme-ultraviolet light. 

Magnets hold cards to your fridge, and store data in your computer. They can power speakers, and produce detailed medical images. And yet, despite millennia of use, and centuries of study, magnetism is still far from fully understood.

The Kapteyn-Murnane group has come up with a novel way to use fast bursts of extreme ultraviolet light to capture how strongly electrons interact with each other in materials. This research is important for figuring out how quickly materials can change their state from insulating to conducting, or from magnetic to nonmagnetic. In the future such fast switching may lead to faster and more efficient nanoelectronics.

Dennis Gardner and his coworkers in the Kapteyn-Murnane group accomplished two major breakthroughs in imaging tiny structures much too small to be seen with visible light microscopes: (1) for the first time in the extreme ultraviolet (EUV) or soft X-ray region, they achieved a resolution smaller than the wavelength of the light; and (2) for the first time, they obtained high resolution quantitative imaging of near periodic tiny objects (structures with repetitive features).

The Kapteyn/Murnane group has measured how long it takes an electron born into an excited state inside a piece of nickel to escape from its birthplace. The electron’s escape is related to the structure of the metal. The escape is the fastest material process that has been measured before in the laboratory––on a time scale of a few hundred attoseconds, or 10^-18 s. This groundbreaking experiment was reported online in Scienceon June 2, 2016. Also in Science on July 1, 2016, Uwe Bovensiepen and Manuel Ligges offered important insights into the unusual significance of this work. 

Cong Chen and his colleagues in the Kapteyn/Murnane group have generated one of the most complex coherent light fields ever produced using attosecond (10-18 s) pulses of circularly polarized extreme ultraviolet (EUV) light. (The circularly polarized EUV light is shown as rotating blue sphere on the left of the picture. The complex coherent light field is illustrated with the teal, lilac, and purple structures along the driving laser beam (wide red line).

Imagine laser-like x-ray beams that can “see” through materials––all the way into the heart of atoms. Or, envision an exquisitely controlled four-dimensional x-ray microscope that can capture electron motions or watch chemical reactions as they happen. Such exquisite imaging may soon be possible with laser-like x-rays produced on a laboratory optical table. These possibilities have opened up because of new research from the Kapteyn/Murnane group.

The Kapteyn/Murnane group, with Visiting Fellow Charles Durfee, has figured out how to use visible lasers to control x-ray light! The new method not only preserves the beautiful coherence of laser light, but also makes an array of perfect x-ray laser beams with controlled direction and polarization. Such pulses may soon be used for observing chemical reactions or investigating the electronic motions inside atoms. They are also well suited for studying magnetic materials and chiral molecules like proteins or DNA that come in left- and right-handed versions.

For decades after the invention of the red ruby laser in 1960, bright laser-like beams were confined to the infrared, visible, and ultraviolet region of the spectrum. Today there’s an exciting revolution afoot: new coherent x-ray beams are now practical, including the EUV beams gracing the cover of the May 1, 2015, special issue of Science honoring the International Year of Light. The same issue features an article entitled “Beyond Crystallography: Diffractive Imaging Using Coherent X-ray Light Sources” that celebrates the revolutionary advances in both large- and small-scale coherent x-ray sources that are transforming imaging in the 21st century.

One of the great challenges in the semiconductor and electronics industries is that as nanoscale features get smaller and processes get faster, enormous amounts of heat need to be quickly carried away from the nanostructures. The Kapteyn/Murnane group has made the counter-intuitive discovery that it is easier to cool these nanostructures when they are arranged closely together. The researchers also developed a theory to explain this unexpected new behavior.

Until recently, researchers who wanted to understand how magnetic materials work had to reserve time on a large, stadium-sized X-ray machine called a synchrotron. Synchrotrons can produce X-ray beams that can be sculpted very precisely to capture how the spins in magnetic materials work together to give us beautiful and useful magnetic properties – for example to store data in a computer hard drive. But now, thanks to Patrik Grychtol and his colleagues in the Kapteyn/Murnane group, there’s a way to conduct this kind of research in a small university laboratory.

Mid-infrared (mid-IR) laser light is accomplishing some remarkable things at JILA. This relatively long-wavelength light (2–4 µm), when used to drive a process called high-harmonic generation, can produce bright beams of soft x-rays with all their punch packed into isolated ultrashort bursts. And, all this takes place in a tabletop-size apparatus. The soft x-rays bursts have pulse durations measured in tens to hundreds of attoseconds (10^-18 s).

Capturing and controlling the fleeting dance of electrons as they rearrange during a chemical reaction has been a long-standing challenge in science for several decades. Since electrons are much lighter than atoms, they can respond almost instantaneously – on time scales of hundreds of attoseconds, where an attosecond is 10^-18 s.

Many people are familiar with the beautiful harmonies created when two sound waves interfere with each other, producing a periodic and repeating pattern that is music to our ears. In a similar fashion, two interfering x-ray waves may soon make it possible to create the fastest possible strobe light ever made. This strobe light will blink fast enough to allow researchers to study the nuclei of atoms and other incredibly tiny structures. The new strobe light is actually very fast coherent laser-like radiation created by the interference of high-energy x-ray waves.

When research associate Wei Xiong and graduate student Dan Hickstein studied quantum dots by shining laser light on them in the gas phase, they got some surprising results. The tiny chunks of material responded differently to series of two laser pulses — depending on their size. Scientists already knew that most of their quantum dots would end up with at least part of an electron wandering around outside of them for some period of time. However, Xiong and his colleagues showed that the electrons from the smallest quantum dots traveled the farthest away.

Graduate student Dan Hickstein (Kapteyn/Murnane group) recently investigated the behavior of electrons ripped from atoms and molecules by intense infrared laser pulses. He and his colleagues collected the liberated electrons onto a detector where they formed intricate patterns that looked a lot like giant spiders. 

The Kapteyn/Murnane group had the idea that it might be possible to produce bright, laser-like beams of x-rays using an ultrafast laser that fits on a small optics table. It was one of those “it probably can’t be done, but we have to try” moments that motivated them to put together a team that includes the Becker theory group, and 16 collaborators in New York, Austria, and Spain. The lead scientist on this effort, Dr. Tenio Popmintchev, was most concerned about the possibility of an explosion, because to generate x-rays at high photon energies, the laser needed to be focused into a fiber containing high-density helium gas at pressures as high as 80 atmospheres. Eighty atmospheres is 80 times the normal air pressure at sea level.

The Kapteyn/Murnane group and scientists from NIST Boulder and Germany have figured out how the interaction of an ultrafast laser with a metal alloy of iron and nickel destroys the metal’s magnetism. In a recent experiment, the researchers were able to observe how individual bits of quantum mechanical magnetization known as “spin” behaved after the metal was heated with the laser.

Predrag Ranitovic dreams of controlling chemical reactions with ultrafast lasers. Now he and his colleagues in the Kapteyn/Murnane group are one step closer to bringing this dream into reality. The group recently used a femtosecond infrared (IR) laser and two extreme ultraviolet (XUV) harmonics created by the same laser to either ionize helium atoms or prevent ionization, depending on experimental conditions. The researchers adjusted experimental conditions to manipulate the electronic structure of the helium atoms as well as control the phase and amplitude of the XUV laser pulses.

The vision of a tabletop x-ray laser has taken a giant step into reality, thanks to Tenio Popmintchev, Ming-Chang Chen and their colleagues in the Kapteyn/Murnane group. By focusing a femtosecond laser into a gas, Popmintchev and Chen generated many colors of x-rays at once, in a band that stretched from the extreme ultraviolet into the soft x-ray region of the electromagnetic spectrum, spanning wavelengths of ranging from about 6 to 2.5 nm. This broad x-ray band has so many different colors that all the waves can be added together to form the shortest strobe light in existence.

If you want to understand how chemical reactions happen, the ability to monitor dynamic positions of atoms in a molecule is critical. There's a well-known laser technique known as coherent Raman spectroscopy that uses a scattering laser pulse to set atoms vibrating and then measures the color shift of reflected light to detect vibration patterns. This technique has been used as a molecular fingerprinting device for simple motions of a molecule.

When Richard Sandberg and his colleagues in the Kapteyn/Murnane group developed a lensless x-ray microscope in 2007 (see JILA Light & Matter, Winter 2008), they were delighted with their ability to obtain a stick-figure image (below) that was comparable in resolution to one from a scanning-electron microscope. 

Imagine being able to observe how a magnet works at the nanoscale level, both in space and in time. For instance, how fast does a nanoscale magnetic material switch its orientation? What if understanding magnetic switching might lead to the use of the spin of an electron rather than its charge to create new devices? A new method for investigating such possibilities is just beginning to be explored.

Heat does not always flow as rapidly near nanostructures as it typically does in solids. Instead, it can go ballistic! Ballistic heat transfer occurs near a tiny device if its size is smaller than the distance a phonon, or lattice vibration, travels before colliding with another phonon. When this happens, heat flow is reduced, and a nanoscale hot spot is created. Ballistic heat transfer away from a hot spot can be as much as three times less efficient than ordinary heat diffusion.

An oxygen molecule (O₂) doesn't fall apart so easily — even when an X-ray knocks out one of its electrons and superexcites the molecule during a process called photoionization. In this process, the X-ray first removes an electron from deep inside the molecule, leaving a hole in O₂+. Then, an outer electron can fall into the hole, and a second outer electron gets ejected, carrying away any excess energy. The loss of the second electron is known as autoionization, or Auger decay.

Researchers in the Kapteyn/Murnane group have decided to use soft X-ray bursts to watch the interplay of electronic and atomic motions inside a molecule. Such information determines how chemical bonds are formed or broken during chemical reactions.

Xibin Zhou and his colleagues in the Kapteyn/Murnane group have come up with a clever new way to study the structure of carbon dioxide (CO₂) and other molecules. The researchers use two innovative tools: (1) coherent electrons knocked out of the CO₂ molecules by a laser and (2) the X-rays produced by these electrons when they re-collide with the same molecules. The coherent electrons and X-rays are produced in a process known as high harmonic generation.

The Kapteyn/Murnane group recently proved that you don’t need an accelerator facility to make the X-Rays for an X-Ray microscope. In fact, you can build the whole device on an optical bench — if you use a femtosecond laser to generate coherent X-Rays. The group makes coherent X-Rays by shining the laser into a glass tube filled with argon gas. The argon atoms absorb many low-energy laser photons and spit out high-energy X-Ray photons when they give up the absorbed energy. The X-Ray beam has all the desirable properties of laser light. For example, it does not spread rapidly and can be used to make holograms.

X-rays are notorious for damaging molecules, including those in our bodies. High in the upper atmosphere, X-rays from the Sun break apart simple molecules like nitrogen (N₂) and drive chemical reactions affecting the Earth. For these reasons, it’s important to understand exactly how radiation interacts with, damages, or destroys specific chemicals.

It’s easy to make X-rays. Physicians and dentists make them routinely in their offices with a Roentgen X-ray tube, which emits X-rays every which way — just like a light bulb, which is nothing like a laser.

When illuminated by X-ray and infrared light beams in tandem, electrons can tap dance off a platinum surface because they've actually grabbed a photon from both beams simultaneously. As you might have guessed, there is more going on here than the ordinary photoelectric effect, which Albert Einstein explained more than a century ago. In the photoelectric effect, electrons escape from a solid after absorbing a single photon or bundle of light energy.