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arXiv:2308.16746 · New Journal of Physics

Post-experiment coincidence detection techniques for direct detection of two-body correlations

De-Zhong Cao, Yuehua Su

Published Nov 12, 2025• 1 citation
arXivHTMLPDF

Abstract

Abstract It is one challenge to develop experimental techniques for direct detection of the many-body correlations of strongly correlated electrons, which exhibit a variety of unsolved mysteries. In this article, we present a post-experiment coincidence counting method and propose two post-experiment coincidence detection techniques, post-experiment coincidence angle-resolved photoemission spectroscopy and post-experiment coincidence inelastic neutron scattering. By coincidence detection of two photoelectric processes or two neutron-scattering processes, the post-experiment coincidence detection techniques can detect directly the two-body correlations of strongly correlated electrons in particle-particle channel or two-spin channel. The post-experiment coincidence detection techniques can be implemented upon the pulse -resolved angle-resolved photoemission spectroscopy or inelastic neutron scattering experimental apparatus with pulse photon or neutron source. When implemented experimentally, they will be powerful techniques to study the highly esoteric high-temperature superconductivity and the highly coveted quantum spin liquids.

DOI
10.1088/1367-2630/ae1e77

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•Nov 30, 2017•0 citations
Abstract It is one challenge to develop experimental techniques for direct detection of the many-body correlations of strongly correlated electrons, which exhibit a variety of unsolved mysteries. In this article, we present a post-experiment coincidence counting method and propose two post-experiment coincidence detection techniques, post-experiment coincidence angle-resolved photoemission spectroscopy and post-experiment coincidence inelastic neutron scattering. By coincidence detection of two photoelectric processes or two neutron-scattering processes, the post-experiment coincidence detection techniques can detect directly the two-body correlations of strongly correlated electrons in particle-particle channel or two-spin channel. The post-experiment coincidence detection techniques can be implemented upon the pulse -resolved angle-resolved photoemission spectroscopy or inelastic neutron scattering experimental apparatus with pulse photon or neutron source. When implemented experimentally, they will be powerful techniques to study the highly esoteric high-temperature superconductivity and the highly coveted quantum spin liquids.
Research on strongly correlated electron systems faces a fundamental challenge due to the complex nature of intrinsic many-body correlations. A key strategy to address this challenge lies in advancing experimental methods that can directly probe and elucidate the underlying many-body correlations. In this perspective article, we discuss the theoretically proposed coincidence detection techniques, which are designed to directly measure two-body correlations in various particle-particle and particle-hole channels, with momentum, energy, and/or spatial resolution. We also explore the prospects of these coincidence detection techniques for future theoretical and experimental developments. The successful implementation and refinement of these coincidence detection techniques promise to deliver powerful new approaches for unraveling long-standing puzzles in strongly correlated electron systems, such as the enigmatic mechanism of unconventional superconductivity and the long-sought quantum spin liquids. Furthermore, these coincidence detection techniques will offer powerful new methods to investigate novel phenomena like itinerant magnetism and electronic nematicity in quantum materials.
In the study of strongly correlated electrons, one of the challenging core tasks is to develop the potential techniques for direct detection of the many-body correlations of strongly correlated electrons. The(γ,2e)photoemission technique has been developed to investigate the two-body correlations of the target correlated electrons. In this article, we will focus on this technique for the correlated electrons near the Fermi energy in condensed matter. The coincidence detection probability of the two emitted electrons in the(γ,2e)photoemission measurement is shown to be relevant to a two-body Bethe-Salpeter wave function, which describes the dynamical two-body correlations of the target correlated electrons near the Fermi energy. As the coincidence detection probability involves an electron-electron interaction matrix element, the arbitrary momentum and/or energy transfer due to this electron-electron interaction makes the(γ,2e)photoemission technique fail to reveal the inner-pair structures of the two-body Bethe-Salpeter wave function. However, the center-of-mass momentum and energy of the two-body Bethe-Salpeter wave function can be distinctly resolved. Thus, the(γ,2e)photoemission technique can provide the center-of-mass physics of the two-body correlations of the target correlated electrons. It will be one potential technique to study the center-of-mass physics of the Cooper pairs in superconductor.
In time-resolved photoemission experiments, more than one electron can be emitted from the solid by a single ultrashort pulse. We theoretically demonstrate how correlations between the momenta of outgoing electrons relate to time-dependent two-particle correlations in the solid. This can extend the scope of time- and angle-resolved photoemission spectroscopy to probe superconducting and charge density fluctuations in systems without long-range order, and to reveal their dynamics independent of the electronic gap and thus unrestricted by the energy-time uncertainty. The proposal is illustrated for superconductivity in a BCS model. An impulsive perturbation can quench the gap on ultrafast timescales, while nonequilibrium pairing correlations persist much longer, even when electron-electron scattering beyond mean-field theory is taken into account. There is thus a clear distinction between a dephasing of the Cooper pairs and the thermalization into the normal state. While a measurement of the gap would be blind to such pairing correlations, they can be revealed by the angular correlations in photoemission.
The discovery of high-Tc superconductivity in cuprates in 1986 moved strongly correlated systems from exotic worlds interesting only for pure theorists to the focus of solid-state research. In recent decades, the majority of hot topics in condensed matter physics (high-Tc superconductivity, colossal magnetoresistance, multiferroicity, ferromagnetism in diluted magnetic semiconductors, etc.) have been related to strongly correlated transition metal compounds. The highly successful electronic structure calculations based on density functional theory lose their predictive power when applied to such compounds. It is necessary to go beyond the mean field approximation and use the many-body theory. The methods and models that were developed for the description of strongly correlated systems are reviewed together with the examples of response function calculations that are needed for the interpretation of experimental information (inelastic neutron scattering, optical conductivity, resonant inelastic X-ray scattering, electron energy loss spectroscopy, angle-resolved photoemission, electron spin resonance, and magnetic and magnetoelectric properties). The peculiarities of (quasi-) 0-, 1-, 2-, and 3- dimensional systems are discussed.
The results of electron-photon coincidence experiments have given a new insight into the excitation of atoms by electron impact. This article reviews the way in which this new experimental technique has provided an exacting and fundamental test for the theory of the excitation process. The basic experimental method is first described, and a comprehensive treatment of excitation of the n 1 P states of helium is given. The extension of the technique to the study of excitation of the n=2 states of atomic hydrogen is then presented. Coincidence measurements also provide information on the role of spin in the collision, and this subject is treated in detail for excitation of heavy atoms by both unpolarised and spin-polarised beams of electrons. Finally, the electron-photon coincidence method permits observation of the time evolution of excited atomic states, and this review describes the attempts made to observe quantum beats in the radiative decay.
Describing correlated electron systems has been a major challenge in computational condensed-matter physics. Quantum Monte Carlo, a powerful computational tool for the study of correlated systems, solves electron correlation problems explicitly. It has been taken as a benchmark method for understanding the correlated systems. Instead of making approximations to Hamiltonian, QMC methods work with the wave functions, and the computational cost scales well with the system size. With the development of parallel computing, QMC calculations on large systems are becoming more and more feasible. We have investigated two correlated systems with highly accurate fixed node QMC techniques. The first system is a correlated hydrogen model system near the metal to insulator transition. We have successfully identified the transition point by calculating spin and charge properties and analyzing the low energy Hilbert space. The second one is a strongly correlated Fe/O system. Calculations on the Fe atoms, O atoms, and FeO molecules are conducted with multiple highly accurate many-body techniques. The source of errors has been disentangled by comparing the results of the many body techniques with the experimental results. For the Fe and O atoms, the calculated properties coincide well with previous experimental results. For the basis-based techniques, the performance is mainly limited by the basis set. The calculated equilibrium bond length, excitation energy and vibrational frequency of the FeO molecules are also in close agreement with the known values from previous experiments.