We develop closed expressions for a time-resolved photon counting signal induced by an entangled photon pair in an interferometric spectroscopy setup. Superoperator expressions in Liouville-space are derived that can account for relaxation and dephasing induced by coupling to a bath. Interferometric setups mix matter and light variables non-trivially, which complicates their interpretation. We provide an intuitive modular framework for this setup that simplifies its description. Based on separation between the detection stage and the light-matter interaction processes. We show that the pair entanglement time and the interferometric time-variables control the observed physics time-scale. Only a few processes contribute in the limiting case of small entanglement time with respect to the sample response, and specific contributions can be singled out.
Over the last several decades, entangled photon pairs generated by spontaneous parametric down conversion processes in both second-order and third-order nonlinear optical materials have been intensively studied for various quantum features such as Bell inequality violation and anticorrelation. In an interferometric scheme, anticorrelation results from photon bunching based on randomness when entangled photon pairs coincidently impinge on a beam splitter. Compared with post-measurement-based probabilistic confirmation, a coherence version has been recently proposed using the wave nature of phot…
Over the last several decades, entangled photon pairs generated from \c{hi}^((2)) nonlinear optical materials via spontaneous parametric down conversion processes have been intensively studied for various quantum correlations such as Bell inequality violation and anticorrelation. In a Mach-Zehnder interferometer, the photonic de Broglie wavelength has also been studied for quantum sensing with an enhanced phase resolution overcoming the standard quantum limit. Here, the fundamental principles of quantumness are investigated in an interferometric scheme for controllable quantum correlation not …
Correlated photons inspire abundance of metrology-related platforms, which benefit from quantum (anti-) correlations and outperform their classical-light counterparts. While such demonstrations mainly focus on entanglement, the role of photon exchange-phase and degree of distinguishability have not been widely utilized in quantum-enhanced applications. Using an interferometric setup we show that even at low degree entanglement, when a two-photon wave-function is coupled to matter, it is encoded with a reliable "which pathway?" information. An interferometric exchange-phase-cycling protocol is …
We survey the inclusion of interferometric elements in nonlinear spectroscopy performed with quantum light. Controlled interference of electromagnetic fields coupled to matter can induce constructive or destructive contributions of microscopic coupling sequences (histories) of matter. Since quantum fields do not commute, quantum light signals are sensitive to the order of light-matter coupling sequence. Matter correlation functions are thus imprinted by different field factors, which depend on that order. We identify the associated quantum information obtained by controlling the weights of dif…
Entangled two-photon spectroscopy is expected to provide advantages compared with classical protocols. It is achieved by coherently controlling the spectral properties of energy-entangled photons. We present here an experimental setup that allows the spectral shaping of entangled photons with high resolution. We evaluate its performances by detecting sum frequency generation in a non-linear crystal. The efficiency of the process is compared when performed with classical or entangled light.
Different degrees of freedom of single photons have been entangled and are used as a resource for various quantum technology applications. We present a simple scheme to perform Bell's test and show the violation of CHSH inequality in a path-entangled single photon state using interferometric and its equivalent non-interferometric approach in beam splitter setting. We demonstrate this experimentally by generating and controlling path-entangled state using both, heralded and un-heralded single photons from spontaneous parametric down-conversion. The experimental results we present show the trans…
Two-photon excitation spectroscopy is a nonlinear technique that has gained rapidly in interest and significance for studying the complex energy-level structure and transition probabilities of materials. While the conventional spectroscopy based on tunable classical light has been long established, quantum light provides an alternative way towards excitation spectroscopy with potential advantages in temporal and spectral resolution, as well as reduced photon fluxes. By using a quantum Fourier transform that connects the sum-frequency intensity and N00N-state temporal interference, we present a…
Entangled photon pair excitation and time-frequency-filtered multidimensional photon correlation spectroscopy as a probe for dissipative exciton kinetics
Center for Free-Electron Laser Science CFEL, Deutsches Elektronen-Synchrotron DESY（自由电子激光科学中心，德国电子同步加速器）；University of California, Irvine（加州大学尔湾分校）
A novel method of macroscopically entangled light-pair generation is presented for a quantum laser using randomness-based deterministic phase control of coherent light in a Mach-Zehnder interferometer (MZI). Unlike the particle nature-based quantum correlation in conventional quantum mechanics, the wave nature of photons is applied for collective phase control of coherent fields, resulting in a deterministically controllable nonclassical phenomenon. For the proof of principle, the entanglement between output light fields from an MZI is examined using the Hong-Ou-Mandel-type anticorrelation tec…
Indistinguishability in quantum mechanics is an essential concept to understanding mysterious quantum features such as self-interference of a single photon and two-photon nonlocal correlation. Delayed-choice experiments are for the cause-effect violation via post-measurements of photons in an interferometric system. Recently, a macroscopic version of the delayed-choice experiments has been demonstrated using the classical means of Poisson distributed photons in a noninterfering Mach-Zehnder interferometer (NMZI). Here, a coherence version of the nonlocal correlation is presented using the wave…
In virtual-state spectroscopy, information about the energy-level structure of an arbitrary sample is retrieved by Fourier transforming sets of measured two-photon absorption probabilities of entangled photon pairs where the degree of entanglement and the delay time between the photons have been varied. This works well for simple systems but quickly becomes rather difficult when many intermediate states are involved. We propose and discuss an extension of entangled two-photon absorption spectroscopy that solves this problem by means of repeated measurements at different pump wavelengths. Speci…
We develop an ultrafast frequency-resolved Raman spectroscopy with entangled photons for polyatomic molecules in condensed phases, to probe the electronic and vibrational coherences. Using quantum correlation between the photons, the signal shows the capability of both temporal and spectral resolutions that are not accessible by either classical pulses or the fields without entanglement. We develop a microscopic theory for this Raman spectroscopy, revealing the electronic coherence dynamics which often shows a rapid decay within $\sim$50fs. The heterodyne-detected Raman signal is further devel…
Quantum light is a key resource for promoting quantum technology. One such class of technology aims to improve the precision of optical measurements using engineered quantum states of light. In this study, we investigate transmission measurement of frequency-entangled broadband photon pairs generated via parametric down-conversion with a monochromatic laser. It is observed that state-to-state dynamics in the system under study are temporally resolved by adjusting the path difference between the entangled twin beams when the entanglement time is sufficiently short. The non-classical photon corr…
We propose an extension of coherent control using laser-synthesized free-electron matter waves. In contrast to coherent control schemes exploiting optical coherences to steer the dynamics of matter waves, we analyze the opposite and investigate the control of quantum light emission driven by laser-sculpted coherent free-electron matter waves. We apply this concept to the control of entangled photon-pair emission in electron-atom collisions, in which the incident electron wave packet, colliding with a target atom $B$, is engineered by interferometric resonantly-enhanced multiphoton ionization o…
