Vibrational Hyper-Raman Molecular Spectroscopy with Entangled Photons
Not provided.
SEARCH · Engineering Papers
Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.
Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.
Not provided.
Not Available
Explore the source record for details and available documents.
A high generation rate photon-pair source using a dual element periodically-poled potassium titanyl phosphate (PP KTP) waveguide is described. The photon-pair source features a high pair generation rate, a compact power-efficient package, and continuous wave (CW) or pulsed operation. Characterization and test results are presented. Details and preliminary results of a laboratory free-space QKD experiment with the B92 protocol are also presented.
Explore the source record for details and available documents.
Explore the source record for details and available documents.
Recently, several researchers, including yours truly, have been able to demonstrate theoretically that quantum photon entanglement has the potential to also revolutionize the entire field of optical interferometry, by providing many orders of magnitude improvement in interferometer sensitivity. The quantum entangled photon interferometer approach is very general and applies to many types of interferometers. In particular, without nonlocal entanglement, a generic classical interferometer has a statistical-sampling shot-noise limited sensitivity that scales like 1/Sqrt[N], where N is the number of particles (photons, electrons, atoms, neutrons) passing through the interferometer per unit time. However, if carefully prepared quantum correlations are engineered between the particles, then the interferometer sensitivity improves by a factor of Sqrt[N] (square root of N) to scale like 1/N, which is the limit imposed by the Heisenberg Uncertainty Principle. For optical (laser) interferometers operating at milliwatts of optical power, this quantum sensitivity boost corresponds to an eight-order-of-magnitude improvement of signal to noise. Applications are to tests of General Relativity such as ground and orbiting optical interferometers for gravity wave detection, Laser Interferometer Gravity Observatory (LIGO) and the European Laser Interferometer Space Antenna (LISA), respectively.
Entangled two-photon absorption (ETPA) exhibits a quantum-enhanced two-photon absorption cross-section and a linear scaling with incident power that exceeds classical two-photon absorption (TPA) at low photon flux. Here, we assess the feasibility and applications of ETPA for active plasma spectroscopy. The ETPA-absorbed power for an Ar + species in a helicon plasma scenario is calculated to be as high as 0.6 nW cm −1 along the incident beam path for nondegenerate-entangled photon pairs that are near-resonant with an intermediate level. The ETPA absorption power exceeds classical TPA and Bremsstrahlung emission, a necessary condition for a feasible fluorescence measurement. Applications of ETPA plasma spectroscopy may include trace impurity detection, ground-state excitation, and continuous-wave pumping for high-bandwidth turbulence measurements. Possible benefits of plasma measurements are less harm to optical components with lower incident flux and reduced stray light that can contaminate optical diagnostics.
The transfer of quantum properties and entanglement between photons and matter (transduction) is a major challenge in QIS, especially with regard to networking quantum information processing. In order to overcome this challenge, it is important to know how non-classical light (single or entangled photons) interacts with matter. This project specifically addresses fundamental questions about the interaction of single and entangled photons with molecules and nanostructures to produce electrons with prescribed spin polarizations and pairs of electrons with entangled spins, thus resulting in transduction by addressing two major objectives: (2) In Objective 1, we will investigate the formation of polarization-encoded radical (spin qubit) pairs and molecular triplet states photoexcited by single quantum emitter light sources. (2) In Objective 2, we will demonstrate the use of two entangled photons, generated by spontaneous parametric down conversion (SPDC) or by the coherent biexcitonic states of perovskite NPLs, to produce two entangled radical (spin qubit) pairs or molecular triplet states.
Stimulated-emission tomography (SET) is an excellent tool for characterizing the process of spontaneous parametric down conversion (SPDC), which is commonly used to create pairs of entangled photons for use in quantum information protocols. The use of stimulated emission increases the average number of detected photons by several orders of magnitude compared to the spontaneous process. In a SET measurement, the parametric down conversion is seeded by an intense signal field prepared with specified mode properties rather than by broadband multimodal vacuum fluctuations, as is the case for the spontaneous process. The SET process generates an intense idler field in a mode that is the complex conjugate to the signal mode. In this work we use SET to estimate the joint spatial mode distribution (JSMD) in the Laguerre-Gaussian (LG) basis of the two photons of an entangled photon pair. The pair is produced by parametric down conversion in a beta barium borate (BBO) crystal with type-II phase matching pumped at a wavelength of 405 nm along with a 780 nm seed signal beam prepared in a variety of LG modes to generate an 842 nm idler beam of which the spatial mode distribution is measured. We observe strong idler production and good agreement with the theoretical prediction of its spatial mode distribution. Our experimental procedure should enable the efficient determination of the photon-pair wavefunctions produced by low-brightness SPDC sources and the characterization of high-dimensional entangled-photon pairs. Published by the American Physical Society 2024
Significance Entangled two-photon absorption has attracted considerable interest due to its potential applications for low–photon flux spectroscopy and microscopy. The entanglement parameters in the twin-photon state can be exploited to control two-photon excitation processes. Here we demonstrate that photon entanglement provides a powerful novel control knob for the nuclear wave packets in an optically dark electronic state. We show that the transition states in the trans–cis photoisomerization of azobenzene, initiated by an entangled two-photon absorption process, can be manipulated significantly by entangled light. These effects can be monitored experimentally by coherent stimulated X-ray Raman signals which reveal electronic coherences during the passage through conical intersections.
The experimental realization of quantum molecular spectroscopy with entangled photons remains challenging owing to the low signal-to-noise ratio resulting from the use of low-flux entangled photons. High-flux entangled photons via intense entangled beams can be used to improve the signal-to-noise ratio, but the presence of unentangled photons contaminates the quantum signal stemming from entangled photons. Here, we demonstrate how intense entangled beams can be used in multi-dimensional spectroscopy while retaining the advantage of photon entanglement. Our approach is broadly applicable to odd-ordered nonlinear spectroscopies, and it generates purely quantum spectroscopic signals. The proposed approach allows the recording of desired phase-matched signals even in a collinear beam geometry, which lifts the requirement of complicated beam geometry setups for phase matching in multi-dimensional spectroscopies.
We report how the unique temporal and spectral features of pulsed entangled photons from a parametric downconversion source can be utilized for manipulating electronic excitations through the optimization of their spectral phase. A new comprehensive optimization protocol based on Bayesian optimization has been developed in this work to selectively excite electronic states accessible by two-photon absorption. Using our optimization method, the entangled two-photon absorption probability for a thiophene dendrimer can be enhanced by up to a factor of 20, while classical light turns out to be nonoptimizable. Moreover, the optimization involving photon entanglement enables selective excitation that would not be possible otherwise. In addition to optimization, we have explored entangled two-photon absorption in the small entanglement time limit showing that entangled light can excite molecular electronic states that are vanishingly small for classical light. As a result, we demonstrate these opportunities with an application to a thiophene dendrimer.
As a follow-up to our previous report on quantum sensing for safeguards, here we delve deeper into quantum-enhanced imaging & spectroscopy and address their relevance to international safeguards. Much of the approaches rely on entangled photons, a quantum phenomenon not possible with classical physics, although just correlated photons will work for some applications, such as ghost imaging. We provide a comprehensive survey of quantum approaches, including multiple entangled photon ghost imaging and spectroscopy techniques. Entangled photons for noise reduction are also described, as well as Non-Line-Of-Sight imaging, compressive techniques, and squeezed light. Of particular interest is the generation of entangled photons with large wavelength separation, such as infrared/visible entangled photon pairs. Such entangled pairs would allow interaction with objects in the IR, such as in the molecular “fingerprint” wavelength region, while the recording device captures the visible photons, thus leveraging the high efficiency and lower cost of visible detectors. Unfortunately, entangled x-ray photons are not practical, which would have been useful for safeguards to interrogate shielded materials. Entangled gamma rays are even further beyond reason. We provide our assessment for application of quantum-enhanced imaging & spectroscopy for international safeguards, including suggested improvements to existing IAEA instruments and destructive assay measurements that are done at IAEA lab facilities.
An interdisciplinary quantum communications and sensing research effort has been underway at the NASA Glenn Research Center since the summer of 2000. Researchers in the Communications Technology, Instrumentation and Controls, and Propulsion and Turbomachinery Divisions have been working together to study and develop techniques that use the principle of quantum entanglement (QE). This work is supported principally by the Nanotechnology Base R&T program at Glenn. As applied to communications and sensing, QE is an emerging technology that holds promise as a new and innovative way to communicate faster and farther, and to sense, measure, and image environmental properties in ways that are not possible with existing technology. Quantum entangled photons are "inseparable" as described by a wave function formalism. For two entangled photons, the term "inseparable" means that one cannot describe one photon without completely describing the other. This inseparability gives rise to what appears as "spooky," or nonintuitive, behavior because of the quantum nature of the process. For example, two entangled photons of lower energy can be created simultaneously from a single photon of higher energy in a process called spontaneous parametric down-conversion. Our research is focused on the use of polarization-entangled photons generated by passing a high-energy (blue) photon through a nonlinear beta barium borate crystal to generate two red photons that have orthogonal, but entangled, polarization states. Although the actual polarization state of any one photon is not known until it is measured, the act of measuring the polarization of one photon completely determines the polarization state of its twin because of entanglement. This unique relationship between the photons provides extra information about the system. For example, entanglement makes it easy to distinguish entangled photons from other photons impinging on a detector. For many other applications, ranging from quantum computation and information to quantum sensing, the entanglement property is critical.
The scalability of quantum networking will benefit from quantum and classical communications coexisting in shared fibers, the main challenge being spontaneous Raman scattering noise. We investigate the coexistence of multi-channel O-band quantum and C-band classical communications. We characterize multiple narrowband entangled photon pair channels across 1282 nm-1318 nm co-propagating over 48 km of installed standard fiber with record C-band power (>18 dBm) and demonstrate that some quantum-classical wavelength combinations significantly outperform others. We analyze the Raman noise spectrum, optimal wavelength engineering, multi-photon pair emission in entangled photon-classical coexistence, and evaluate the implications for future quantum applications.
Multiphoton absorption of entangled photons offers ways for obtaining unique information about chemical and biological processes. Measurements with entangled photons may enable sensing biological signatures with high selectivity and at very low light levels to protect against photodamage. In this paper, we present a theoretical and experimental study of the excitation wavelength dependence of the entangled two-photon absorption (ETPA) process in a molecular system, which provides insights into how entanglement affects molecular spectra. We demonstrate that the ETPA excitation spectrum can be different from that of classical TPA as well as that for one-photon resonant absorption (OPA) with photons of doubled frequency. These results are modeled by assuming the ETPA cross-section is governed by a two-photon excited state radiative linewidth rather than by electron-phonon interactions, and this leads to excitation spectra that match the observed results. Further, we find that the two-photon-allowed states with highest TPA and ETPA intensities have high electronic entanglements, with ETPA especially favoring states with the longest radiative lifetimes. These results provide concepts for the development of quantum light–based spectroscopy and microscopy that will lead to much higher efficiency of ETPA sensors and low-intensity detection schemes.