With a microwave-regime cyclic three-state configuration, an enantiomer-selective state transfer~(ESST) is carried out through the two-path interference between a direct one-photon coupling and an effective two-photon coupling. The $π$-phase difference in the one-photon process between two enantiomers makes the interference constructive for one enantiomer but destructive for the other. Therefore only one enantiomer is excited into a higher rotational state while the other remains in the ground state. The scheme is of flexibility in the pulse waveforms and the time order of two paths. We simulate the scheme in a sample of cyclohexylmethanol~(C$_7$H$_{14}$O) molecules. Simulative results show the robust and high-fidelity ESST can be obtained when experimental concerns are considered. Finally, we propose to employ the finished ESST in implementing enantio-separation and determining enantiomeric excess.
Microwave three-wave mixing allows for enantiomer-selective excitation of randomly oriented chiral molecules into rotational states with different energy. The random orientation of molecules is reflected in the degeneracy of the rotational spectrum with respect to the orientational quantum number $M$ and reduces, if not accounted for, enantiomer-selectivity. Here, we show how to design pulse sequences with maximal enantiomer-selectivity from an analysis of the $M$-dependence of the Rabi frequencies associated with rotational transitions induced by resonant microwave drives. We compare differen…
Molecular matter-wave interferometry enables novel strategies for manipulating the internal mechanical motion of complex molecules. Here, we show how chiral molecules can be prepared in a quantum superposition of two enantiomers by far-field matter-wave diffraction and how the resulting tunnelling dynamics can be observed. We determine the impact of ro-vibrational phase averaging and propose a setup for sensing enantiomer-dependent forces, parity-violating weak interactions, and environment-induced superselection of handedness, as suggested to resolve Hund's paradox. Using ab-initio tunnelling…
State-selective enantiomeric excess is realized using microwave-driven coherent population transfer. The method selectively promotes either R or S molecules to a higher rotational state by phase-controlled microwave pulses that drive electric-dipole allowed rotational transitions. We demonstrate the enantiomer-specific state transfer method using enantiopure samples of 1,2-propanediol. This method of state-specific enantiomeric enrichment can be applied to a large class of asymmetric, chiral molecules that can be vaporized and cooled to the point where rotationally resolved spectroscopy is pos…
We prove complete controllability for rotational states of an asymmetric top molecule belonging to degenerate values of the orientational quantum number M. Based on this insight, we construct a pulse sequence that energetically separates population initially distributed over degenerate M-states, as a precursor for orientational purification. Introducing the concept of enantio-selective controllability, we determine the conditions for complete enantiomer-specific population transfer in chiral molecules and construct pulse sequences realizing this transfer for population initially distributed ov…
We present an optical "enantio-selective switch", that, in two steps, turns a ("racemic") mixture of left-handed and right-handed chiral molecules into the enantiomerically pure state of interest. The optical switch is composed of an "enantio-discriminator" and an "enantio-converter" acting in tandem. The method is robust, insensitive to decay processes, and does not require molecular preorientation. We demonstrate the method on the purification of a racemate of (transiently chiral) D$_2$S$_2$ molecules, performed on the nanosecond timescale.
The relations between quantum coherence and quantum interference are discussed. A general method for generation of quantum coherence through interference-induced state selection is introduced and then applied to `simple' atomic systems under two-photon transitions, with applications in quantum optics and laser cooling.
We present a comprehensive study of enantioselective orientation of chiral molecules excited by a pair of delayed cross-polarized femtosecond laser pulses. We show that by optimizing the pulses' parameters, a significant (~ 10%) degree of enantioselective orientation can be achieved at zero and at five kelvin rotational temperatures. This study suggests a set of reasonable experimental conditions for inducing and measuring strong enantioselective orientation. The strong enantioselective orientation and the wide availability of the femtosecond laser systems required for the proposed experiments…
Three-wave mixing spectroscopy of chiral molecules, which exist in left-handed and right-handed conformations, allows for enantio-selective population transfer despite random orientation of the molecules. This is based on constructive interference of the three-photon pathways for one enantiomer and destructive one for the other. We prove here that three mutually orthogonal polarization directions are required to this end. Two different dynamical regimes exist to realize enantio-selective population transfer, and we show that they correspond to different phase conditions in the three-wave mixin…
A quantum-eraser experiment is reported with photon pairs generated by two synchronously pumped parametric down converters coupled via induced coherence. The complementarity between which-source information and two-photon interference fringe visibility has been investigated by two coupled interferometers.
We theoretically analyze the observations reported in a four-path quantum interference experiment via multiple beam Ramsey interference [Phys. Rev. Lett. 86, 559 (2001)]. In this experiment, a selective scattering of photons from just one interfering path causes decoherence. However, contrary to expectations, there is an increase in the contrast of the interference pattern, demonstrating that path selective decoherence can not only lead to a decrease, but under certain conditions, to an increase of the fringe contrast. Here we explain this seemingly counter-intuitive effect based on a model fo…
Differing from the traditional method of achieving subwavelength interference, we have demonstrated the two-photon subwavelength interference effect of broadband chaotic light in a polarization-selective Michelson interferometer with an ultrafast two-photon absorption detector the first time, which is achieved by manipulating two-photon probability amplitudes involved in the interference. In theory, the two-photon polarization coherence matrix and probability amplitudes matrix are combined to develop polarized two-photon interference terms, which explains the experimental results well. In orde…
Frequency encoding of quantum information together with fiber and integrated photonic technologies can significantly reduce the complexity and resource requirements for realizing all-photonic quantum networks. The key challenge for such frequency domain processing of single photons is to realize coherent and selective interactions between quantum optical fields of different frequencies over a range of bandwidths. Here, we report frequency-domain Hong-Ou-Mandel interference with spectrally distinct photons generated from a chip-based microresonator. We use four-wave mixing to implement an activ…
We report an electrically driven semiconductor single photon source capable of emitting photons with a coherence time of up to 400 ps under fixed bias. It is shown that increasing the injection current causes the coherence time to reduce and this effect is well explained by the fast modulation of a fluctuating environment. Hong-Ou-Mandel type two-photon interference using a Mach-Zehnder interferometer is demonstrated using this source to test the indistinguishability of individual photons by post-selecting events where two photons collide at a beamsplitter. Finally, we consider how improvement…
Mode-selective nonlinear interference for high-brightness and high-purity fiber-coupled SPDC sources
Fraunhofer Institute for Applied Optics and Precision Engineering（弗劳恩霍夫应用光学和精密工程研究所）；Friedrich Schiller University Jena, Institute of Applied Physics, Abbe Center of Photonics（耶拿弗里德里希·席勒大学应用物理学院阿贝光子学中心）
Enantiosensitive exceptional points in open chiral systems
Max-Born-Institut（马克斯·玻恩研究所）；Attosecond Quantum Physics Laboratory, Physics Department, King’s College London（伦敦国王学院物理学院阿秒量子物理实验室）；Technion-Israel Institute of Technology（以色列理工学院）；Institute of Advanced Studies in Theoretical Chemistry, Technion-Israel Institute of Technology（以色列理工学院理论化学高级研究所）；Department of Physics, Humboldt Universität zu Berlin（柏林洪堡大学物理系）；Department of Physics, Imperial College London（伦敦帝国理工学院物理系）；Technische Universität Berlin（柏林工业大学）
Based on constructive interference in Sagnac waveguide loop, an efficient scheme is proposed for selective frequency conversion and multifrequency modes W entanglement via input-output formalism. We can adjust the probability amplitudes of output photons by choosing parameter values properly. The tunable probability amplitude will lead to the generation of output photon with a selectable frequency and W photonic entanglement of different frequencies modes in a wide range of parameter values. Our calculations show the present scheme is robust to the deviation of parameters and spontaneous decay…
We demonstrate full selective control over the constructive or destructive character of fourth-order recurring interferences in a modified version of a HOM interferometer using comb-like two-photon states. The comb spectral/temporal structure is obtained by inserting an etalon cavity in the signal path of an entangled photon pair obtained by pulsed spontaneous parametric down-conversion. Both a simple qualitative discussion and a complete theoretical derivation are used to explain and analyze the experimental data.
We numerically show that time delayed coherent feedback controls the statistical output characteristics of driven quantum emitters. Quantum feedback allows to enhance or suppress a wide range of classical and nonclassical features of the emitted quantum light. As exemplary quantum system, we use a pumped cavity containing two emitters. By applying phase-selective feedback, we demonstrate that photon antibunching and bunching can be increased in orders of magnitude due to intrinsically and externally controllabe quantum interferences. Our modelling is based on a fully non-Markovian quantum simu…
The interference pattern of the resonance fluorescence from a J=1/2 to J=1/2 transition of two identical atoms confined in a three-dimensional harmonic potential is calculated. Thermal motion of the atoms is included. Agreement is obtained with experiments [Eichmann et al., Phys. Rev. Lett. 70, 2359 (1993)]. Contrary to some theoretical predictions, but in agreement with the present calculations, a fringe visibility greater than 50% can be observed with polarization-selective detection. The dependence of the fringe visibility on polarization has a simple interpretation, based on whether or not…
We present a method that implement directional, perfect state transfers within a branched spin network by exploiting quantum interferences in the time-domain. That provides a tool to isolate subsystems from a large and complex one. Directionality is achieved by interrupting the spin-spin coupled evolution with periods of free Zeeman evolutions, whose timing is tuned to be commensurate with the relative phases accrued by specific spin pairs. This leads to a resonant transfer between the chosen qubits, and to a detuning of all remaining pathways in the network, using only global manipulations. A…
We propose an enantio-detection method of chiral molecules in a cavity with external drive. The chiral molecules are coupled with a quantized cavity field and two classical light fields to form the cyclic three-level systems. The chirality-dependent cavity-assisted three-photon process in the three-level systems leads to the generation of intracavity photons. Simultaneously, the drive field also results in the chirality-independent process of the generation of intracavity photons. Based on the interference between the intracavity photons generated from these two processes, one can detect the e…
We investigate optimal states of photon pairs to excite a target transition in a multilevel quantum system. With the help of coherent control theory for two-photon absorption with quantum light, we infer the maximal population achievable by optimal entangled vs. separable states of light. Interference between excitation pathways, as well as the presence of nearby states, may hamper the selective excitation of a particular target state, but we show that quantum correlations can help to overcome this problem, and enhance the achievable "selectivity" between two energy levels, i.e. the relative d…
We report on the state of the art of quantum walk experiments with neutral atoms in state-dependent optical lattices. We demonstrate a novel state-dependent transport technique enabling the control of two spin-selective sublattices in a fully independent fashion. This transport technique allowed us to carry out a test of single-particle quantum interference based on the violation of the Leggett-Garg inequality and, more recently, to probe two-particle quantum interference effects with neutral atoms cooled into the motional ground state. These experiments lay the groundwork for the study of dis…
The phenomenon of "overlapping resonances interference-induced transparency" (ORIT) is introduced and studied in detail for the $S_0 \to S_2/S_1$ photoexcitation of cold pyrazine (C$_4$H$_4$N$_2$). In ORIT a molecule becomes transparent at specific wavelengths due to interferences between envelopes of spectral lines displaying overlapping resonances. An example is the $S_2\leftrightarrow S_1$ internal conversion in pyrazine where destructive interference between overlapping resonances causes the $S_0 \to S_2/S_1$ light absorption to disappear at certain wavelengths. ORIT may be of practical im…
We experimentally demonstrate the generation of heralded bi-chromatic single photons from an atomic collective spin excitation (CSE). The photon arrival times display collective quantum beats, a novel interference effect resulting from the relative motion of atoms in the CSE. A combination of velocity-selective excitation with strong laser dressing and the addition of a magnetic field allows for exquisite control of this collective beat phenomenon. The present experiment uses a diamond scheme with near-IR photons that can be extended to include telecommunications-wavelengths or modified to all…
