Optical nonlinearities typically require macroscopic media, thereby making their implementation at the quantum level an outstanding challenge. Here we demonstrate a nonlinearity for one atom enclosed by two highly reflecting mirrors. We send laser light through the input mirror and record the light from the output mirror of the cavity. For weak laser intensity, we find the vacuum-Rabi resonances. But for higher intensities, we find an additional resonance. It originates from the fact that the cavity can accommodate only an integer number of photons and that this photon number determines the characteristic frequencies of the coupled atom-cavity system. We selectively excite such a frequency by depositing at once two photons into the system and find a transmission which increases with the laser intensity squared. The nonlinearity differs from classical saturation nonlinearities and is direct spectroscopic proof of the quantum nature of the atom-cavity system. It provides a photon-photon interaction by means of one atom, and constitutes a step towards a two-photon gateway or a single-photon transistor.
Photon coincidence spectroscopy relies on detecting multiphoton emissions from the combined atom-cavity system in atomic beam cavity quantum electrodynamics experiments. These multiphoton emissions from the cavity are nearly simultaneous approximately on the cavity lifetime scale. We determine the optimal time for the detection window of photon pairs in two-photon coincidence spectroscopy. If the window time is too short, some photon pairs will not be detected; if the window time is too long, too many nearly coincident independent single photons will be falsely interpreted as being a photon pa…
Photon coincidence spectroscopy is a promising technique for probing the nonlinear regime of cavity quantum electrodynamics in the optical domain, however its accuracy is mitigated by two factors: higher-order photon correlations, which contribute to an enhanced pair count rate, and non-simultaneity of emitted photon pairs from the optical cavity. We show that the technique of photon coincidence spectroscopy is effective in the presence of these effects if the quantitative predictions are adjusted to include non-simultaneity and higher-order correlations.
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 show that photon coincidence spectroscopy can provide an unambiguous signature of two atoms simultaneously interacting with a quantised cavity field mode. We also show that the single-atom Jaynes-Cummings model can be probed effectively via photon coincidence spectroscopy, even with deleterious contributions to the signal from two-atom events. In addition, we have explicitly solved the eigenvectors and eigenvalues of two two-level atoms coupled to a quantised cavity mode for differing coupling strengths.
We experimentally demonstrate optical spectroscopy of magnetically trapped atoms on an atom chip. High resolution optical spectra of individual trapped clouds are recorded within a few hundred milliseconds. Detection sensitivities close to the single atom level are obtained by photoionization of the excited atoms and subsequent ion detection with a channel electron multiplier. Temperature and decay rates of the trapped atomic cloud can be monitored in real time for several seconds with only little detection losses. The spectrometer can be used for investigations of ultracold atomic mixtures an…
Quantum spectroscopy was performed using the frequency-entangled broadband photon pairs generated by spontaneous parametric down-conversion. An absorptive sample was placed in front of the idler photon detector, and the frequency of signal photons was resolved by a diffraction grating. The absorption spectrum of the sample was measured by counting the coincidences, and the result is in agreement with the one measured by a conventional spectrophotometer with a classical light source.
We present the computation of two-photon transition spectra between ro-vibrational states of the H2+ molecular ion, including the effects of hyperfine structure and excitation polarization. The reduced two-photon matrix elements are obtained by means of a variational method. We discuss the implications of our results for high-resolution spectroscopy of H2+.
Non-equilibrium photon correlations of coherently excited single quantum systems can reveal their internal quantum dynamics and provide spectroscopic access. Here we propose and discuss the fundamentals of a coherent photon coincidence spectroscopy based on the application of laser pulses with variable delay and the detection of an time-averaged two-photon coincidence rate. For demonstration, two simple but important cases, i.e., an exciton - biexciton in a quantum dot and two coupled quantum emitters, are investigated based on quantum dynamics simulations demonstrating that this nonlinear spe…
We investigate Ramsey spectroscopy performed on a synchronized ensemble of two-level atoms. The synchronization is induced by the collective coupling of the atoms to a heavily damped mode of an optical cavity. We show that, in principle, with this synchronized system it is possible to observe Ramsey fringes indefinitely, even in the presence of spontaneous emission and other sources of individual-atom dephasing. This could have important consequences for atomic clocks and a wide range of precision metrology applications.
We propose a feasible experimental scheme, employing methods of population spectroscopy with two-level atoms, for a test of Bell's inequality for massive particles. The correlation function measured in this scheme is the joint atomic $Q$ function. An inequality imposed by local realism is violated by any entangled state of a pair of atoms.
Atomic spectroscopy, an essential tool for frequency estimation, is widely used in quantum sensing. Atom-atom interaction can be used to generate entanglement for achieving quantum enhanced sensing. However, atom-atom interaction always induces collision shift, which brings systematic error in determining the resonance frequency. Contradiction between utilizing atom-atom interaction and suppressing collision shift generally exists in atomic spectroscopy. Here, we propose an antisymmetric Rabi spectroscopy protocol without collision shift in the presence of atom-atom interactions. We analytical…
It is shown that spectrally resolved photon-statistics measurements of the resonance fluorescence from realistic semiconductor quantum-dot systems allow for high contrast identification of the two-photon strong-coupling states. Using a microscopic theory, the second-rung resonance is analyzed and optimum excitation conditions are determined. The computed photon-statistics spectrum displays gigantic, experimentally robust resonances at the energetic positions of the second-rung emission.
We perform a high resolution Fourier Transform Spectroscopy of optical sources in the few-photon regime based on the phenomenon of two-photon interference in a beam splitter. From the heterodyne interferogram between test and reference sources it is possible to obtain the spectrum of the test source relative to that of the reference. The method proves to be a useful asset for spectral characterization of faint optical sources below the range covered by classical heterodyne beating techniques.
We show that shifts in locations of two-photon coincidence spectral peaks, for a bichromatically-driven two-level atom passing through a single-mode cavity, are due to competition between excitation pathways for a Jaynes-Cummings system. We also discuss an analogous shift of (single-photon) spectral peaks for a driven three-level V-system, which demonstrates that competition between excitation pathways is also important in this simple system.
We report on the collapse and revival of Ramsey fringe visibility when a spatially dependent phase is imprinted in the coherences of a trapped ensemble of two-level atoms. The phase is imprinted via the light shift from a Gaussian laser beam which couples the dynamics of internal and external degrees of freedom for the atoms in an echo spectroscopy sequence. The observed revivals are directly linked to the oscillatory motion of atoms in the trap. An understanding of the effect is important for quantum state engineering of trapped atoms.
We describe and characterize a setup for subrecoil stimulated Raman spectroscopy of cold cesium atoms. We study in particular the performances of a method designed to active control and stabilization of the magnetic fields across a cold-atom cloud inside a small vacuum cell. The performance of the setup is monitored by {\em copropagative-beam} stimulated Raman spectroscopy of a cold cesium sample. The root mean-square value of the residual magnetic field is 300 $μG$, with a compensation bandwidth of 500 Hz. The shape of the observed spectra is theoretically interpreted and compares very well t…
It is controversial what is the true role of entanglement in two-photon virtual-state spectroscopy [Saleh et al, Phys. Rev. Lett. 80, 3483, 1998], a two-photon absorption spectroscopic technique that can retrieve information about the energy level structure of an atom or a molecule. The consideration of closely related techniques, such as multidimensional pump-probe spectroscopy [Roslyak et al, Phys. Rev. A 79, 063409, 2009], might suggest that spectroscopic information retrieved in the two-photon absorption process is the same regardless of the classical or quantum nature of the light source.…
Traditionally, spectroscopy is performed by examining the position of absorption lines. However, at frequencies near the transition frequency, additional information can be obtained from the phase shift. In this work we consider the information about the transition frequency obtained from both the absorption and the phase shift, as quantified by the Fisher information in an interferometric measurement. We examine the use of multiple single-photon states, NOON states, and numerically optimized states that are entangled and have multiple photons. We find the optimized states that improve over th…
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…
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…
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 propose a relatively robust scheme to generate maximally entangled states of (i) an atom and a cavity photon, (ii) two atoms in their ground states, and (iii) two photons in two spatially separate high-Q cavities. It is based on the interaction via fractional adiabatic passage of a three-level atom traveling through a cavity mode and a laser beam. The presence of optical phases is emphasized.
We extend the analysis of photon coincidence spectroscopy beyond bichromatic excitation and two-photon coincidence detection to include multichromatic excitation and multiphoton coincidence detection. Trichromatic excitation and three-photon coincidence spectroscopy are studied in detail, and we identify an observable signature of a triple resonance in an atom-cavity system.
Fourier transform spectroscopy with classical interferometry corresponds to the measurement of a single-photon intensity spectrum from the viewpoint of the particle nature of light. In contrast, the Fourier transform of two-photon quantum interference patterns provides the intensity spectrum of the two photons as a function of the sum or difference frequency of the constituent photons. This unique feature of quantum interferometric spectroscopy offers a different type of spectral information from the classical measurement and may prove useful for nonlinear spectroscopy with two-photon emission…
Single-shot high-resolution spectroscopy of single-photon-level optical pulses using a virtually imaged phased-array and single-photon avalanche diode array
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）
We demonstrate a method to perform spectroscopy of near-infrared single photons without the need of dispersive elements. This method is based on a photon energy resolving transition edge sensor and is applied for the characterization of widely wavelength tunable narrow-band single photons emitted from a crystalline whispering gallery mode resonator. We measure the emission wavelength of the generated signal and idler photons with an uncertainty of up to 2 nm.
We discuss a recently demonstrated type of microwave spectroscopy of trapped ultra-cold atoms known as "echo spectroscopy" [M.F. Andersen et. al., Phys. Rev. Lett., in press (2002)]. Echo spectroscopy can serve as an extremely sensitive experimental tool for investigating quantum dynamics of trapped atoms even when a large number of states are thermally populated. We show numerical results for the stability of eigenstates of an atom-optics billiard of the Bunimovich type, and discuss its behavior under different types of perturbations. Finally, we propose to use special geometrical constructio…
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…
We propose and demonstrate a method for measuring the joint spectrum of photon pairs via Fourier spectroscopy. The biphoton spectral intensity is computed from a two-dimensional interferogram of coincidence counts. The method has been implemented for a type-I downconversion source using a pair of common-path Mach-Zender interferometers based on Soleil compensators. The experimental results agree well with calculated frequency correlations that take into account the effects of coupling into single-mode fibers. The Fourier method is advantageous over scanning spectrometry when detectors exhibit …
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$50fs. The heterodyne-detected Raman signal is further devel…
In photon recoil spectroscopy, signals are extracted from recoils imparted by the spectroscopy light on the motion of trapped ions as demonstrated by C. Hempel et al., Nature Photonics 7, 630 (2013) and Y. Wan et al., Nature Communications 5, 3096 (2014). The method exploits the exquisite efficiency in the detection of phonons achievable in ion crystals, and is thus particularly suitable for species with broad non-cycling transitions where detection of fluorescence photons is impractical. Here, we develop a theoretical model for the description of photon recoil spectroscopy based on a Fokker-P…
The erbium atomic system is a promising candidate for an atomic Bose-Einstein condensate of atoms with a non-vanishing orbital angular momentum ($L \neq 0$) of the electronic ground state. In this paper we report on the frequency stabilization of a blue external cavity diode laser system on the 400.91 $nm$ laser cooling transition of atomic erbium. Doppler-free saturation spectroscopy is applied within a hollow cathode discharge tube to the corresponding electronic transition of several of the erbium isotopes. Using the technique of frequency modulation spectroscopy, a zero-crossing error sign…
The energy-level structure of a single atom strongly coupled to the mode of a high-finesse optical cavity is investigated. The atom is stored in an intracavity dipole trap and cavity cooling is used to compensate for inevitable heating. Two well-resolved normal modes are observed both in the cavity transmission and the trap lifetime. The experiment is in good agreement with a Monte Carlo simulation, demonstrating our ability to localize the atom to within $λ/10$ at a cavity antinode.
We demonstrate Faraday spectroscopy with high duty cycle and sampling rate using atoms confined to a blue-detuned optical trap. Our trap consists of a crossed pair of high-charge-number hollow laser beams, which forms a dark, box-like potential. We have used this to measure transient magnetic fields in a 500-micron-diameter spot over a 400 ms time window with nearly unit duty cycle at a 500 Hz sampling rate. We use these measurements to quantify and compensate time-varying magnetic fields to ~10 nT per time sample.
Remote Infrared Absorption Spectroscopy with Undetected Photons
Université Marie et Louis Pasteur, CNRS, institut FEMTO-ST（玛丽和路易·巴斯德大学，法国国家科学研究中心，FEMTO-ST研究所）；Group of Applied Physics, University of Geneva（日内瓦大学应用物理组）
Precision spectroscopy of atomic and molecular ions offers a window to new physics, but is typically limited to species with a cycling transition for laser cooling and detection. Quantum logic spectroscopy has overcome this limitation for species with long-lived excited states. Here, we extend quantum logic spectroscopy to fast, dipole-allowed transitions and apply it to perform an absolute frequency measurement. We detect the absorption of photons by the spectroscopically investigated ion through the photon recoil imparted on a co-trapped ion of a different species, on which we can perform ef…
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…
A spectroscopic application of the atom laser is suggested. The spectroscopy termed 2PACC employs the coherent properties of matter-waves from a two pulse atom laser. These waves are employed to control a gas-surface chemical recombination reaction. The method is demonstrated for an Eley-Rideal reaction of a hydrogen or alkali atom-laser pulse where the surface target is an adsorbed hydrogen atom. The reaction yields either a hydrogen or alkali hydride molecule. The desorbed gas phase molecular yield and its internal state is shown to be controlled by the time and phase delay between two atom-…
We investigate the prospects of using two-mode intensity squeezed twin-beams, generated in Rb vapor, to improve the sensitivity of spectroscopic measurements by engaging two-photon Raman transitions. As a proof of principle demonstration, we demonstrated the quantum-enhanced measurements of the Rb $5D_{3/2}$ hyperfine structure with reduced requirements for the Raman pump laser power and Rb vapor number density.
Terahertz spectroscopy allows for identifying different isomers of materials, for drug discrimination as well as for detecting hazardous substances. As many dielectric materials used for packaging are transparent in the terahertz spectral range, substances might even be identified if packaged. Despite these useful applications, terahertz spectroscopy suffers from the still technically demanding detection of terahertz radiation. Thus, either coherent time-domain-spectroscopy schemes employing ultrafast pulsed lasers or continuous-wave detection with photomixers requiring two laser systems are u…
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.
Optical signals obtained by the material response to classical laser fields are given by nonlinear response functions which can be expressed by sums over various quantum pathways of matter. We show that some pathways can be selected by using nonclassical fields, through the entanglement of photon and material pathways, which results in a different-power law dependence on the incoming field intensity. Spectrally overlapping stimulated Raman scattering (SRS) and two-photon-absorption (TPA) pathways in a pump probe experiment are separated by controlling the degree of entanglement of pairs of inc…
Exploring the interaction of light and matter at the ultimate limit of single photons and single emitters is of great interest both from a fundamental point of view and for emerging applications in quantum engineering. However, the difficulty of generating single photons with specific wavelengths, bandwidths and brightness as well as the weak interaction probability of a single photon with an optical emitter pose a formidable challenge toward this goal. Here, we demonstrate a general approach based on the creation of single photons from a single emitter and their use for performing spectroscop…
We perform spectroscopy on the hyperfine splitting of $^{85}$Rb atoms trapped in far-off-resonance optical traps. The existence of a spatially dependent shift in the energy levels is shown to induce an inherent dephasing effect, which causes a broadening of the spectroscopic line and hence an inhomogeneous loss of atomic coherence at a much faster rate than the homogeneous one caused by spontaneous photon scattering. We present here a number of approaches for reducing this inhomogeneous broadening, based on trap geometry, additional laser fields, and novel microwave pulse sequences. We then sh…
The excited state population of single solid-state emitters is subjected to energy fluctuations around the equilibrium driven by the bath and relaxation through the emission of phonons or photons. Simultaneous measurement of the associated spectral dynamics requires a technique with a high spectral and temporal resolution with an additionally high temporal dynamic range. We propose a pulsed excitation-laser analog of Photon-Correlation Fourier Spectroscopy (PCFS), which extracts the lineshape and spectral diffusion dynamics along the emission lifetime trajectory of the emitter, effectively dis…
Atoms in highly excited (Rydberg) states have a number of unique properties which make them attractive for applications in quantum information. These are large dipole moments, lifetimes and polarizabilities, as well as strong long-range interactions between Rydberg atoms. Experimental methods of laser cooling and precision spectroscopy enable the trapping and manipulation of single Rydberg atoms and applying them for practical implementation of quantum gates over qubits of a quantum computer based on single neutral atoms in optical traps. In this paper, we give a review of the experimental and…
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…
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…
