Justin C. Goodrich, Ryan Mahon, Joseph Hanrahan, Dennis Bollweg, Monika Dziubelski, Raphael A. Abrahão, Sanjit Karmakar, K. Gofron, Thomas A Caswell, Daniel Allan, Lonny E. Berman, ANDREI NOMEROTSKI, Andrei Fluerasu, C. Da Vià, Sean M. McSweeney
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.
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.
Quantum imaging leverages correlations between pairs of photons and has the potential to obtain image information beyond what classical sources provide. Extending this approach to the X-ray regime has been limited by low photon-pair generation rates and the lack of suitable detectors. Here, we demonstrate X-ray coincidence imaging using spontaneous parametric down-conversion (SPDC) and a pixelated area detector with time- and energy-resolved capabilities. This configuration enables simultaneous detection of correlated X-ray photon pairs and coincidence-based imaging of test objects, including a biological specimen. The increased coincidence rate and spatially resolved detection establish a basis for future quantum-enhanced and low-dose X-ray imaging.
Spontaneous parametric down-conversion is a vital method for generating correlated photon pairs in the visible and near-infrared spectral regions; however, its extension to X-ray frequencies has faced substantial barriers. Here, we present an advancement in correlated X-ray pair generation and detection by employing a two-dimensional pixelated detector to obtain the first direct image of the pair distribution. Our study explores and directly visualizes the down-conversion process, revealing the characteristic ring structure of coincident photon pairs and demonstrating robust spatial correlations. A significant finding is the observation of energy anti-correlation, achieved at an unprecedented rate of approximately 4,100 pairs/hour, far exceeding previous reports in the literature. We believe these results represent a significant leap in X-ray quantum imaging, unlocking the potential for enhanced imaging of biological materials with reduced doses and broadening the applicability of X-ray quantum optical technologies.
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.
The process of image recording is arguably one of the most prevalent technology in modern society and continues to inspire vast swathes of research due to its widespread applications spanning military, medical and consumer spheres. The danger present in a field so broad is that separate niches of research can become isolated with critical advancements struggling to traverse the gulfs between. Unifying the field is the omnipresent drive to acquire an ever increasing quality of images at the lowest possible cost, a goal which warrants continual fundamental research. Quantum entanglement exhibits many intriguing characteristics which make it a suitable tool for such fundamental investigations. The process of spontaneous parametric down- conversion has offered a yet unbeaten strength of photon correlations with the quantum nature of their production providing a reliable and controllable source of single-photons. Arising from these attributes is the technique known as ghost imaging. Though now known to be classically possible, the strength of entanglement generated correlations is yet to be surpassed. This thesis implemented this technique in tandem with the cutting edge detector technology in order to probe the fundamentals of image formation. This form of imaging allowed us to subject an object to a known number of photons whilst acquiring structural information from spatially separate, correlated photons which never interact with the object. The strength of the produced correlations allow us to acquire low background, high resolution images with far less light than traditional techniques and affords many novel benefits. The possibility of incorporating this technique with pre-existent regimes allowed me to draw from advancements made across the landscape of imaging research. Although referred to as “quantum ghost imaging” throughout this work, it should be noted that the intrinsic quantum nature of the correlations was not directly relied upon but provided an ideal source of strongly correlated photons. In order to determine the limits of a traditional imaging system this thesis first sought to answer the question: “can an image of an object be reconstructed from fewer photons than ii pixels in the image?” In chapter 3 I approached this from the perspective of compression, which minimises redundant information within a signal. This lead to the development of an imaging regime capable of imaging with far fewer photons than pixels in the image. By employing assumptions about the sparsity of natural images I was able to reconstruct an image of a biological sample containing an average of less than one photon per image pixel. Having reduced the number of photons necessary to form an image I then considered alternative methods for reducing the optical energy impinging on a sample. I sought to answer the question: “can non-degenerate ghost imaging reduce the optical energy impinged upon an object during imaging”. The photons produced in SPDC need not be of similar wavelengths, however may be chosen far from degeneracy, i.e. non-degenerate. In Chapter 4 I presented a ghost imaging system which illuminated the object with infrared light whilst recording the structural information via entangled visible photons. This allowed for objects opaque to visible light to be imaged in high quality without the need for a spatially resolving infrared detector, the state of the art of which lags behind their silicon based visible counterparts. I presented the systems capabilities by imaging objects which were etched into a gold substrate layered on to silicon, both of which are opaque to visible light. Not only did a reduction in energy deposition arise from the lower energy probe wavelength but applying the reconstruction techniques from the previous chapter brought that down to as low as ≈16 nJcm−2s−1. Seeking to expand the repertoire of applications, the low-light capabilities of my ghost imaging were applied to the technique of phase-contrast microscopy in chapter 5. Typically applied to translucent objects, phase-contrast imaging transfers phase information, i.e. the refractive index changed within the object, into an intensity distribution through the use of a phase-filter. In many of these applications the objects tend to be biological in nature, where high optical exposure can result in bleaching or damage. By applying the phase-filter non- locally, i.e. to the photons correlated to those probing the object, I acquired edge-enhanced images of a phase object whilst illuminating with significantly fewer photons than standard phase-contrast techniques. Having displayed the broad applicability of our low-light ghost imaging system, I then sought to determine the optical resolution in chapter 6. The resolution limits of ghost imaging are not clear at first glance owing to the resolutions dependence upon the strength of spatial correlations. As the length over which the spatial correlations are produced can be brought below the standard diffraction limit, it would seem the resolution of the system could be brought similarly low. To clarify this I artificially restricted the number of spatial modes in each of the correlated beams to uncover the physically realisable resolution. I show that although the resolution of a ghost imaging system to be fundamentally determined by the strength of the correlations, this can never be reached due to the inherent limitations of the intervening imaging system.
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 leverages nonclassical correlations to reveal features that may vanish in conventional event integration [ 1, 2]. While single-photon detectors are well-established, quantum imaging demands complex data acquisition across many thousands of detectors, each generating rich metadata including triggering time, duration, and other properties. Consequently, effective data management, data wrangling, and correlation extraction become critical challenges. In this work, we investigate optimal handling of spatial correlations from a quantum-photonic source (spontaneous parametric down-conversion, SPDC) using an emerging single-photon event-based camera, the TPX3CAM (256×256 array, supported by an intensifier). Utilizing a femtosecond photon-pair source, we comprehensively analyse noise characteristics, including temporal dynamics and spatial distribution, to develop advanced spatio-temporal noise suppression strategies tailored to camera performance. Our primary objectives include real-time isolation and preprocessing of correlative data. Our analysis demonstrates the potential of these real-time correlation detection and noise reduction algorithms to expand quantum imaging capabilities across diverse scientific domains. Potential applications include high-resolution spectroscopy in biology, materials science, and advanced electron microscopy, where these techniques could enable identification of cascaded two-photon processes with atomic-scale precision. Figure 1 shows an excellent example of such a detection in real-space. The ring feature corresponds to the location of the correlated photon-pairs produced from the SPDC process. This is also apparent in figure 2, where we see a strong anti-correlation between the coordinates of the detected photons – corresponding to photon-pairs. <!-- named anchor --> Figure 1: Distribution of SPDC photons on TPX3CAM <!-- named anchor --> Figure 2: Spatial anti-correlation of x-coordinates