Clocking the movement of electrons inside an atom

January 22, 2021

Clocking the movement of electrons inside an atom

Artistic depiction of the experiment featuring self-referenced attosecond streaking
Scientists dramatically enhance the achievable resolution at X-ray free-electron lasers with new technique

Hard X-ray free-electron lasers (XFELs) have delivered intense, femtosecond X-ray pulses for over a decade. More recently, even attosecond XFEL pulses have become available, cementing these facilities’ importance for ultrafast science.

One of the most promising applications of XFELs is in biology, where researchers can capture images down to the atomic scale before the radiation damage destroys the sample. In physics and chemistry, these X-rays can also shed light on the fastest processes occurring in nature with a shutter speed lasting only one femtosecond — equivalent to a millionth of a billionth of a second.

However, on these miniscule timescales, it is extremely difficult to synchronize the X-ray pulse that sparks a reaction in the sample with the laser pulse that observes it. This problem — timing jitter —  is a major hurdle in efforts to perform time-resolved experiments at XFELs with ever-shorter time resolution.

Louis DiMauro
Now, a large international research team involving collaborators from Ohio State, DESY in Hamburg, PSI in Switzerland and many other institutions across seven countries has found a solution to this problem, demonstrating its efficacy by measuring a fundamental fast-decay process in an atom. The work was published recently in Nature Physics. The experiments were conducted using the Linear Coherent Light Source (LCLS) XFEL at the SLAC National Accelerator Laboratory in Menlo Park, California.
Yu Hang Lai
The Ohio State team included Hagenlocker Chair and professor in the Department of Physics Louis DiMauro, physics postdoctoral researcher Yu Hang Lai and former physics research scientist Cosmin Blaga, now an assistant professor of physics at Kansas State University.

Many biological systems — and some non-biological ones — suffer damage when excited by X-rays. One cause of damage known as Auger decay occurs when the X-ray pulse catapults core-level electrons in the sample out of place, leading to their replacement by electrons in outer shells. As these outer electrons relax, they release energy, which can induce the emission of another electron, known as an Auger electron. Radiation damage is caused by both the X-rays and the continued emission of Auger electrons, which can rapidly degrade the sample. Timing this decay helps evade radiation damage.

Ordinarily, timing jitter would appear to preclude time-resolved studies of such a short process at an XFEL. To circumvent the jitter, the research team came up with a pioneering, highly precise approach to chart Auger decay. The technique, self-referenced attosecond streaking, is based on mapping the electrons in thousands of images and deducing when they were emitted.

For the first application of this method, the team used neon gas, where the decay timings have been inferred in the past. After exposing both types of emitted electrons to an external streaking laser pulse, the researchers determined their final kinetic energy in each of tens of thousands of individual measurements. Crucially, in each measurement, the Auger electrons always interact with the streaking laser pulse slightly later than the photoelectrons. This constant factor forms the foundation of the technique. By combining so many individual observations, the team was able to construct a detailed map of the physical process, thereby determining the characteristic time delay between the photo- and Auger-emission.

The researchers hope that self-referenced streaking will have a broader impact in the field of ultrafast science. Essentially, the technique enables traditional attosecond streaking spectroscopy, previously restricted to tabletop sources, to be extended to XFELs worldwide as they approach the attosecond frontier. In this way, self-referenced streaking may facilitate a new class of experiments benefitting from the flexibility and extreme intensity of XFELs without compromising on time resolution.

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