Abstract Optical interferometry has been a long-standing setup for characterization of quantum states of light. Both linear and the nonlinear interferences can provide information regarding the light statistics and underlying detail of the light-matter interactions. Here we demonstrate how interferometric detection of nonlinear spectroscopic signals may be used to improve the measurement accuracy of matter susceptibilities. Light-matter interactions change the photon statistics of quantum light, which are encoded in the field correlation functions. Application is made to the Hong-Ou-Mandel two-photon interferometer that reveals entanglement-enhanced resolution that can be achieved with existing optical technology.
Abstract Optical interferometry has been a long-standing setup for characterization of quantum states of light. Both linear and the nonlinear interferences can provide information regarding the light statistics and underlying detail of the light-matter interactions. Here we demonstrate how interferometric detection of nonlinear spectroscopic signals may be used to improve the measurement accuracy of matter susceptibilities. Light-matter interactions change the photon statistics of quantum light, which are encoded in the field correlation functions. Application is made to the Hong-Ou-Mandel two-photon interferometer that reveals entanglement-enhanced resolution that can be achieved with existing optical technology.
Entangled photon pairs have been used for molecular spectroscopy in the form of entangled two-photon absorption and in quantum interferometry for precise measurements of light source properties and time delays. We present an experiment that combines molecular spectroscopy and quantum interferometry by utilizing the correlations of entangled photons in a Hong-Ou-Mandel (HOM) interferometer to study molecular properties. We find that the HOM signal is sensitive to the presence of a resonant organic sample placed in one arm of the interferometer, and the resulting signal contains information pertaining to the light-matter interaction. We can extract the dephasing time of the coherent response induced by the excitation on a femtosecond time scale. A dephasing time of 102 fs is obtained, which is relatively short compared to times found with similar methods and considering line width broadening and the instrument entanglement time As the measurement is done with coincidence counts as opposed to simply intensity, it is unaffected by even-order dispersion effects, and because interactions with the molecular state affect the photon correlation, the observed measurement contains only these effects and no other classical losses. The experiments are accompanied by theory that predicts the observed temporal shift and captures the entangled photon joint spectral amplitude and the molecule's transmission in the coincidence counting rate. Thus, we present a proof-of-concept experimental method based of entangled photon interferometry that can be used to characterize optical properties in organic molecules and can in the future be expanded on for more complex spectroscopic studies of nonlinear optical properties.
Quantum interferences of entangled photons have engendered tremendous intriguing phenomena that lack any counterpart in classical physics. Hitherto, owing to the salient properties of quantum optics, quantum interference has been widely studied and provides useful tools that ultimately broaden the path towards ultra-sensitive quantum metrology, ranging from sub-shot-noise quantum sensing to high-resolution optical spectroscopy. In particular, quantum interferometric metrology is an essential requisite for extracting information about the structure and dynamics of photon-sensitive biological and chemical molecules. This article reviews the theoretical and experimental progress of this quantum interferometric metrology technology along with their advanced applications. The scope of this review includes Hong–Ou–Mandel interferometry with ultrahigh timing resolution, entanglement-assisted absorption spectroscopy based on a Fourier transform, and virtual-state spectroscopy using tunable energy-time entangled photons.
Absorption spectroscopy has long been hailed as an absolute necessity for detecting the properties of complex chemical and biological samples. While conventional spectroscopy using classical light is severely limited by shot noise and lacks robustness against experimental imperfections, quantum light offers an avenue to perform absorption spectroscopy with provable advantages in the technical operations and the measurement precision. Here, we present an experimental approach to implement entanglement-based absorption spectroscopy with the assistance of Hong-Ou-Mandel interference. Since the temporal interference fringe is determined by the spectrum pattern, a maximum-likelihood decision is sufficient for revealing the relevant quantum information about the absorptive properties of the test samples. These experimental results may significantly facilitate the use of quantum interferometric spectroscopy to practical applications, which may be particularly relevant for photon-sensitive biological and chemical samples.
We introduce optical lock-in detection in coincidence photon counting to enhance the extraction of information in “quantum-light spectroscopy”, based on using time-frequency entangled photon pairs to probe a molecular sample. The sample is placed inside a Mach-Zehnder interferometer, into which photons are injected and detected in coincidence at the interferometer output. Clear signatures of two-photon interference (both ‘Hong-Ou-Mandel’ and ‘N00N’) are observed and separated into distinct information channels. In addition to achieving an increased signal-to-noise ratio (SNR) at low count rates, the experiment uses a “down-sampling” technique that increases the efficiency of data collection by an order of magnitude.
Conspectus The enhanced interest in quantum-related phenomena has provided new opportunities for chemists to push the limits of detection and analysis of chemical processes. As some have called this the second quantum revolution, a time has come to apply the rules learned from previous research in quantum phenomena toward new methods and technologies important to chemists. While there has been great interest recently in quantum information science (QIS), the quest to understand how nonclassical states of light interact with matter has been ongoing for more than two decades. Our entry into this field started around this time with the use of materials to produce nonclassical states of light. Here, the process of multiphoton absorption led to photon-number squeezed states of light, where the photon statistics are sub-Poissonian. In addition to the great interest in generating squeezed states of light, there was also interest in the formation of entangled states of light. While much of the effort is still in foundational physics, there are numerous new avenues as to how quantum entanglement can be applied to spectroscopy, imaging, and sensing. These opportunities could have a large impact on the chemical community for a broad spectrum of applications. In this Account, we discuss the use of entangled (or quantum) light for spectroscopy as well as applications in microscopy and interferometry. The potential benefits of the use of quantum light are discussed in detail. From the first experiments in porphyrin dendrimer systems by Dr. Dong-Ik Lee in our group to the measurements of the entangled two photon absorption cross sections of biological systems such as flavoproteins, the usefulness of entangled light for spectroscopy has been illustrated. These early measurements led the way to more advanced measurements of the unique characteristics of both entangled light and the entangled photon absorption cross-section, which provides new control knobs for manipulating excited states in molecules. The first reports of fluorescence-induced entangled processes were in organic chromophores where the entangled photon cross-section was measured. These results would later have widespread impact in applications such as entangled two-photon microscopy. From our design, construction and implementation of a quantum entangled photon excited microscope, important imaging capabilities were achieved at an unprecedented low excitation intensity of 10 7 photons/s, which is 6 orders of magnitude lower than the excitation level for the classical two-photon image. New reports have also illustrated an advantage of nonclassical light in Raman imaging as well. From a standpoint of more precise measurements, the use of entangled photons in quantum interferometry may offer new opportunities for chemistry research. Experiments that combine molecular spectroscopy and quantum interferometry, by utilizing the correlations of entangled photons in a Hong–Ou–Mandel (HOM) interferometer, have been carried out. The initial experiment showed that the HOM signal is sensitive to the presence of a resonant organic sample placed in one arm of the interferometer. In addition, parameters such as the dephasing time have been obtained with the opportunity for even more advanced phenomenology in the future.
We provide a comprehensive analysis of the reconstruction of the density matrix for entangled photon pairs, utilizing polarization measurements within a Hong-Ou-Mandel (HOM) interference framework. The purpose of this study is to develop a new efficient approach for quantum state characterization, leveraging quantum interference to reduce wave dispersion and utilizing the maximum likelihood method for density matrix reconstruction. The model involves projecting the entangled photons onto a set of sixteen unique polarization states, enabling the observation of detailed quantum interference patterns. We use these patterns to reconstruct the density matrix, revealing the system’s quantum state and degree of entanglement. Our findings demonstrate the effectiveness of this method in accurately characterizing the quantum state of light, while leveraging quantum interference to reduce wave dispersion and improve signal quality and resolution. Our study underscores the effectiveness of this method in accurately characterizing the quantum state of light and highlights the essential role of precise density matrix reconstruction in a Hong-Ou-Mandel interferometer without the use of polarizers. The methodology and results presented lay a strong foundation for further research, with implications for improving measurement accuracy and exploring more complex quantum systems in various quantum information applications. • Density matrix of entangled photon pairs using Hong-Ou-Mandel interference profiles. • Quantum interference and density matrix improve signal quality. • Density matrix is reconstructed using HOM interference and maximum likelihood. • Theoretical study on quantum state reconstruction and its role in quantum information.