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Optica

X-ray parametric down-conversion at an XFEL

N. J. Hartley, James Baxter, Scott Curtis, Okhura Daisuke, Aliaksei Halavanau, Abigail Hardy Carpenter, Janita Hussain, Taito Osaka, Norimasa Ozaki, Richard Lunt Sandberg, S. Shwartz, Kai Taketoshi, Naoki Yamagata, Siegfried Heinz Glenzer

Published May 19, 2025• 4 citations
Publisher

Abstract

Understanding and harnessing X-ray quantum effects could open new, to our knowledge, frontiers in imaging and quantum optics. In this study, we measured the process of X-ray parametric down-conversion, where a single high-energy X-ray photon splits into two lower-energy photons. Using the SACLA X-ray free electron laser in Japan at 9.83 keV, we found clear evidence that pairs of photons were produced along the energy-angle relationship that conserved both energy and momentum, as predicted for down-conversion, and consistent with quantum entanglement of X-ray photons. By matching specific photon pairs for energy and momentum conservation, we observe a signal rate of 1250 pairs per hour, confirming that correlated photon pairs can be generated and observed in the absence of explicit time correlations. Our results show that with further refinement, the number of entangled photons produced per laser pulse could increase by an order of magnitude. This paves the way for demonstrating quantum-enhanced X-ray imaging, and confirmation of X-ray photon entanglement.

DOI
10.1364/optica.560275

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Understanding and harnessing X-ray quantum effects could open new, to our knowledge, frontiers in imaging and quantum optics. In this study, we measured the process of X-ray parametric down-conversion, where a single high-energy X-ray photon splits into two lower-energy photons. Using the SACLA X-ray free electron laser in Japan at 9.83 keV, we found clear evidence that pairs of photons were produced along the energy-angle relationship that conserved both energy and momentum, as predicted for down-conversion, and consistent with quantum entanglement of X-ray photons. By matching specific photon pairs for energy and momentum conservation, we observe a signal rate of 1250 pairs per hour, confirming that correlated photon pairs can be generated and observed in the absence of explicit time correlations. Our results show that with further refinement, the number of entangled photons produced per laser pulse could increase by an order of magnitude. This paves the way for demonstrating quantum-enhanced X-ray imaging, and confirmation of X-ray photon entanglement.
Quantum imaging encompasses a broad range of methods that exploit the quantum properties of light to capture information about an object. One such approach involves using a two-photon quantum state, where only one photon interacts with the object being imaged while its entangled partner carries spatial or temporal information. To implement this technique, it is necessary to generate specific quantum states of light and detect photons at the single-photon level. While this method has been successfully demonstrated in the visible electromagnetic spectrum, extending it to X-rays has faced significant challenges due to the difficulties in producing a sufficient rate of X-ray photon pairs and detecting them with adequate resolution. Here, we demonstrate record high rates of correlated X-ray photon pairs produced via a spontaneous parametric down-conversion process and we employ these photons to perform quantum correlation imaging of several objects, including a biological sample (E. cardamomum seedpod). Notably, we report an unprecedented detection rate of about 6,300 pairs per hour and the observation of energy anti-correlation for the X-ray photon pairs. We also present a detailed analysis of the properties of the down-converted X-ray photons, as well as a comprehensive study of the correlation imaging formation, including a study of distortions and corrections. These results mark a substantial advancement in X-ray quantum imaging, expanding the possibilities of X-ray quantum optical technologies, and illustrating the pathway towards enhancing biological imaging with reduced radiation doses.
Abstract Einstein, Podolsky and Rosen's prediction on incompleteness of quantum mechanics was overturned by experimental tests on Bell's inequality that confirmed the existence of quantum entanglement. In X-ray optics, entangled photon pairs can be generated by X-ray parametric down conversion (XPDC), which is limited by relatively low efficiency. Meanwhile, free electron laser (FEL) has successfully lased at X-ray frequencies recently. However, FEL is usually seen as a classical light source, and its quantum effects are considered minor corrections to the classical theory. Here we investigate entangled X-ray photon pair emissions in FEL. We establish a theory for coherently amplified entangled photon pair emission from microbunched electron pulses in the undulator. We also propose an experimental scheme for the observation of the entangled photon pairs via energy and spatial correlation measurements. Such an entangled X-ray photon pair source is of great importance in quantum optics and other X-ray applications.
Imaging with X-rays poses fundamental limits due to radiation damage of the highly energetic photons. This becomes problematic for sensitive biological systems such as subcellular structures. Lowering the radiation dose, without sacrificing the signal-to-noise ratio, would be desirable for any kind of imaging modalities involving X-rays. To achieve this goal, quantum imaging with entangled X-ray photons constitutes a promising route. Production of biphotons have been demonstrated in the X-ray regime by the process of Spontaneous Parametric Down-Conversion (SPDC). However, compared to SPDC in the regime of visible light, the production rate for X-ray biphotons is extremely low. With the introduction of new high average brightness X-ray sources, such as 4th generation synchrotrons and high repetition rate Free-Electron X-ray Lasers (XFEL), quantum imaging may become practical. We introduce a ray tracing approach using Monte-Carlo sampling, specifically designed for quantum imaging with entangled X-ray photons generated by SPDC. By simulation, the superior image quality of quantum over classical imaging methods is demonstrated using realistic experimental conditions available at high repetition rate XFELs. With these simulations, we can efficiently assist the design of future experiments at beam lines, which can substantially accelerate the advancement of X-ray quantum imaging and reduce costs.
We present the first experimental demonstration of quantum enhanced detection at x-ray wavelengths.We show that x-ray pairs that are generated by spontaneous down-conversion can be used for the generation of heralded x-ray photons and directly measure the sub-Poissonian statistics of the single photons by using photon number resolving detectors.We utilize the properties of the strong time-energy correlations of the down-converted photons to demonstrate the ability to improve the visibility and the signal-to-noise ratio of an image with a small number of photons in an environment with a noise level that is higher than the signal by many orders of magnitude.A long-term goal of this work is to demonstrate x-ray photon entanglement.However, given the technical challenges, which are much greater than in the visible regime, we take a first step in demonstrating nonclassical (sub-Poisson) photon correlations.In our work, we demonstrate a new protocol for the measurement of quantum effects with x rays using advantages such as background-free measurements that the x-ray regime offers for experiments aiming at testing fundamental concepts in quantum optics.
We directly observe far-field correlations of x-ray photon pairs generated by spontaneous parametric down-conversion (SPDC). Using an energy-resolved, two-dimensional photon counting detector we record the full ring-shaped emission of both photons across a broad bandwidth and extract pair correlations directly from raw events without imposing angular constraints. The ring radii scale with photon energy, in quantitative agreement with transverse phase matching, providing a stringent momentum-space validation of x-ray SPDC. These observations open a route to leveraging quantum correlations in x-ray imaging and metrology, including correlation-enhanced magnification and reduced blurring.