We introduce the concept of initial-phase spectroscopy as a control of the dynamics of entangled states encoded into a two-atom system interacting with a broadband squeezed vacuum field. We illustrate our considerations by examining the transient spectrum of the field emitted by two systems, the small sample (Dicke) and the spatially extended (non-Dicke) models. It is found that the shape of the spectral components depends crucially on the relative phase between the initial entangled state and the squeezed field. We follow the temporal evolution of the spectrum and show that depending on the relative phase a hole burning can occur in one of the two spectral lines. We compare the transient behavior of the spectrum with the time evolution of the initial entanglement and find that the hole burning can be interpreted as a manifestation of the phenomenon of entanglement sudden death. In addition, we find that in the case of the non-Dicke model, the collective damping rate may act like an artificial tweezer that rotates the phase of the squeezed field.
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.
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 en…
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）
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 numerically analyze the use of intense entangled twin beams for ultra-sensitive spectroscopic measurements in chemical and biological systems. The examined scheme makes use of intense frequency-modulated (chirped) entangled beams to successfully extract information about the intermediate material states that contribute to the two-photon excitation of an absorbing medium. Robustness of the presented method is examined with respect to the applied intervals of the frequency chirp.
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…
In this contribution we analyze virtual-state spectroscopy --- a unique tool for extracting information about the virtual states that contribute to the two-photon excitation of an absorbing medium --- as implemented by means of intense entangled beams with tunable spectral correlations. We provide a thorough description of all contributing terms (classical and quantum) in the two-photon absorption signal, as well as the limits imposed by the power of the pump that produces the entangled beams on the observability of the spectral lines of the virtual transitions. We find that virtual-state spec…
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…
Entangled photons exhibit non-classical light-matter interactions that create new opportunities in materials and molecular science. For example, in entangled two-photon absorption, the intensity-dependence scales linearly as if only one photon was present. The entangled two-photon absorption cross section approaches but does not match the one-photon absorption cross section. The entangled two photon cross section also does not follow classical two photon molecular design motifs. Questions such as these seed the rich but nascent field of entangled light-matter interactions. In this perspective,…
Recent advances in techniques for generating quantum light have stimulated research on novel spectroscopic measurements using quantum entangled photons. One such spectroscopy technique utilizes non-classical correlations among entangled photons to enable measurements with enhanced sensitivity and selectivity. Here, we investigate spectroscopic measurement utilizing entangled three photons. In this measurement, time-resolved entangled photon spectroscopy with monochromatic pumping [J. Chem. Phys. 153, 051102 (2020).] is integrated with the frequency-dispersed two-photon counting technique, whic…
Quantum information science is driving progress in a vast number of scientific and technological areas that cover molecular spectroscopy and matter-light interactions in general. In these fields, the ability to generate quantum mechanically-entangled photons is opening avenues to explore the interaction of molecules with quantum light. This work considers an alternative way of correlating photons by including energy superpositions. We study how the multichromatic quantum superposition, or color superposition of photon-pair states, influences the optical properties of organic chromophores. This…
Optical interferometry has been a long-standing setup for characterization of quantum states of light. Both the linear and the nonlinear interferences can provide information about the light statistics an 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 in…
Entangled two-photon absorption spectroscopy (TPA) has been widely recognized as a powerful tool for revealing relevant information about the structure of complex molecular systems. However, to date, the experimental implementation of this technique has remained elusive, mainly because of two major difficulties. First, the need to perform multiple experiments with two-photon states bearing different temporal correlations, which translates in the necessity to have at the experimenter's disposal tens, if not hundreds, of sources of entangled photons. Second, the need to have \emph{a priori} know…
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 …
The authors demonstrate a form of two-photon-counting interferometry by measuring the coincidence counts between single-photon-counting detectors at an output port of a Mach-Zehnder Interferometer (MZI) following injection of broad-band time-frequency-entangled photon pairs (EPP) generated from collinear spontaneous parametric down conversion into a single input port. Spectroscopy and refractometry are performed on a sample inserted in one internal path of the MZI by scanning the other path in length, which acquires phase and amplitude information about the samples linear response. Phase modul…
While two-photon absorption (TPA) and other forms of nonlinear interactions of molecules with isolated time-frequency-entangled photon pairs (EPP) have been predicted to display a variety of fascinating effects, their potential use in practical quantum-enhanced molecular spectroscopy requires close examination. This paper presents a detailed theoretical study of quantum-enhanced TPA by both photon-number correlations and spectral correlations, including an account of the deleterious effects of dispersion. While such correlations in EPP created by spontaneous parametric down conversion can incr…
Entangled photons offer two advantages for two-photon absorption spectroscopy. One of them, the linear scaling of two-photon absorption rate with the input photon flux, is only valid at very low photon fluxes and is therefore impractical. The other is the overcoming of the classical constraints for simultaneous resolution in time-frequency and in space-wavevector. Here we consider bright squeezed vacuum (BSV) as an alternative to entangled photons. The efficiency increase it offers in comparison with coherent light is modest, but it does not depend on the photon flux. Moreover, and this is wha…
We investigate how entangled inertial Unruh-DeWitt detectors are affected by interaction with a quantum field using a nonperturbative method. Inertial detectors in a $(3+1)$-dimensional Minkowski spacetime with instantaneous switching ($δ$-switching) experience degradation of their initial entanglement as their coupling strength with a scalar field increases. Somewhat surprisingly, initially separable or weakly entangled detectors can extract mutual information from the vacuum. We also find that entanglement degradation is not reduced if communication via the field is possible; rather this onl…
Entangled photon pairs are predicted to linearize and increase the efficiency of two-photon absorption, allowing continuous wave laser diodes to drive ultrafast time-resolved spectroscopy and nonlinear processes. Despite a range of theoretical studies and experimental measurements, inconsistencies persist about the value of the entanglement enhanced interaction cross section. A spectrometer is constructed that can temporally and spectrally characterize the entangled photon state before, during, and after any potential two-photon excitation event. For the molecule Rhodamine 6G, which has a virt…
Generating Entangled Steady States in Multistable Open Quantum Systems via Initial State Control
JILA, NIST, and Department of Physics, University of Colorado（科罗拉多大学物理系、JILA和NIST）；Center for Theory of Quantum Matter, University of Colorado（科罗拉多大学量子物质理论中心）；Department of Applied Mathematics, University of Colorado（科罗拉多大学应用数学系）
We investigate sharing of bipartite entanglement in a scenario where half of an entangled pair is possessed and projectively measured by one observer, called Alice, while the other half is subjected to measurements performed sequentially, independently, and unsharply, by multiple observers, called Bobs. We find that there is a limit on the number of observers in this entanglement distribution scenario. In particular, for a two-qubit maximally entangled initial shared state, no more than twelve Bobs can detect entanglement with a single Alice for arbitrary -- possibly unequal -- sharpness param…
The possibility of generating a multi-hops network between different entangled nodes (qubits) via spin Dipolar interaction is examined. The negativity, tangle and the non-local coherent advantage are used as quantifiers of the generated quantum correlations. The phenomena of the sudden death/birth is displayed for the entangled two nodes, while the sudden changes phenomena (increasing/ decreasing) is depicted for all entangled three nodes. The amount of correlations between the different nodes depend on the initial network settings, where the largest amount is predicted if the network is initi…
我们讨论的技术，允许长的相干时间在激光光谱实验与两个被困离子。我们表明，为了这个目的，不仅纠缠的离子中制备的消相干的子空间可以使用，但也是一对离子，不纠缠，但受到相同的相位噪声。我们将此技术应用于测量~（40）Ca ~（++）3d D ~（5/2）态的电四极矩和测量激发一对~（40）Ca ~（++）离子的超稳激光的线宽。
The problem of conditions on the initial correlations between the system and the environment that lead to completely positive (CP) or not-completely positive (NCP) maps has been studied by various authors. Two lines of study may be discerned: one concerned with families of initial correlations that induce CP dynamics under the application of an arbitrary joint unitary on the system and environment; the other concerned with specific initial states that may be highly entangled. Here we study the latter problem, and highlight the interplay between the initial correlations and the unitary applied.…
