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For theoretically studying molecules with fluorescence in the near-infrared region, high-accuracy determination of state energy level is required for meaningful analyses since the spectra of interest are of very narrow energy range. In particular, these molecules are in many cases handled in solution; therefore, consideration of the solvation effect is essential upon calculation together with the electronic structure of the excited state. Earlier studies showed that they cannot be described with conventional methods such as PCM-TD-DFT, yielding results far from experimental data. Here, we have developed a new method by combining a solvation theory based on statistical mechanics (RISM) and a multireference perturbation theory (CASPT2) with the extension of the density matrix renormalization group reference states for calculating the photochemical properties of near-infrared molecules and have obtained higher-accuracy prediction.

Determination of excited states of near-infrared (NIR) bioimaging dyes is a challenging theoretical task because of their energy levels with a small gap and the presence of solvation. In the previous study, we showed that the development of the reference interaction site model coupled with the complete active space second-order perturbation theory, the RISM-CASPT2 method, and its extension with the density matrix renormalization group enabled high accuracy prediction of the photochemical properties of bioimaging-related fluorescent molecules in solution (Shimizu et al.

Conventional optical synthesis, the manipulation of the phase and amplitude of spectral components to produce an optical pulse in different temporal modes, is revolutionizing ultrafast optical science and metrology. These technologies rely on the Fourier transform of light fields between time and frequency domains in one-dimensional space. However, within this treatment it is impossible to incorporate the quantum correlation among photons. Here we expand the Fourier synthesis into high dimensional space to deal with the quantum correlation, and carry out an experimental demonstration by manipulating the two-photon probability distribution of a biphoton in two-dimensional time and frequency space. As a potential application, we show manipulation of a heralded single-photon wave packet, which is never explained by the conventional one-dimensional Fourier optics. Our approach opens up a new pathway to tailor the temporal characteristics of a biphoton wave packet with high dimensional quantum-mechanical treatment. We anticipate such high dimensional treatment of light in time and frequency domains could bridge the research fields between quantum optics and ultrafast optical measurements., Comment: 12 pages, 7 figures

We experimentally demonstrate a polarization-entangled photon source at 810 nm using a type-II phase-matched periodically poled potassium titanyl phosphate (PPKTP) crystal pumped by a low-cost, broadband laser diode with a central wavelength of 405 nm and a typical bandwidth of 0.53 nm. The PPKTP crystal is placed in a Sagnac loop to realize the compact size and high stability. The downconverted biphotons, the signal and the idler, have typical bandwidths of 5.57 and 7.32 nm. We prepare two Bell states | Ψ + ⟩ and | Ψ − ⟩ with the fidelities of 0.948 ± 0.004 and 0.963 ± 0.002 . In the polarization correlation measurement, the visibilities are all higher than 96.2%, and in the Bell inequality test, the S value can achieve 2.78 ± 0.01 . This high-quality and low-cost entangled photon source may have many practical applications in quantum information processing.

Spectrally intrinsically uncorrelated biphoton states generated from nonlinear crystals are very important but rare resources for quantum photonics and quantum information applications. Previously, such biphoton states were generated from several kinds of crystals, however, their wavelength ranges and nonlinear efficiencies were still limited for various applications. In order to explore new crystal for wider wavelength range and higher nonlinear efficiency, here we theoretically study the generation of spectrally uncorrelated biphoton states from 14 crystals in the `BBO family', including BBO, CLBO, KABO, KBBF, RBBF, CBBF, BABF, BiBO, LBO, CBO, LRB4, LCB, YCOB, and GdCOB. They satisfy three kinds of group-velocity matching condition from near-infrared to telecom wavelengths. Furthermore, heralded single photons can be generated with a purity as high as 0.98, which is achieved without any narrow filtering. The indistinguishability of photons from independent sources is examined by the Hong-Ou-Mandel interference, which results in a visibility of 98% also without any further filtering, i.e., photons from different heralded single-photon sources are highly indistinguishable. Our study may provide single-photon sources with good performance for quantum information processing at near-infrared and telecom wavelengths., Comment: 10 pages, 6 figures

Light incident upon molecules trigger fundamental processes in diverse systems present in nature. However, under natural conditions, such as sunlight illumination, it is impossible to assign known times for photon arrival owing to continuous pumping, and therefore, the photo-induced processes cannot be easily investigated. In this work, we theoretically demonstrate that characteristics of sunlight photons such as photon number statistics and spectral distribution can be emulated through quantum entangled photon pair generated with the parametric down-conversion (PDC). We show that the average photon number of the sunlight in a specific frequency spectrum, e.g., the visible light, can be reconstructed by adjusting the PDC crystal length and pump frequency, and thereby molecular dynamics induced by the pseudo-sunlight can be investigated. The entanglement time, which is the hallmark of quantum entangled photons, can serve as a control knob to resolve the photon arrival times, enabling investigations on real-time dynamics triggered by the pseudo-sunlight photons., Comment: 7 pages

We report a simple scheme for direct generation of frequency-bin entangled photon pairs via spontaneous parametric downconversion. Our fabricated nonlinear optical crystal with two different poling periods can simultaneously satisfy two different, spectrally symmetric nondegenerate quasi-phase-matching conditions, enabling the direct generation of entanglement in two discrete frequency-bin modes. Our produced photon pairs exhibited Hong-Ou-Mandel interference with high-visibility beating oscillations, a signature of two-mode frequency-bin entanglement. Moreover, we demonstrate deterministic entanglement-mode conversion from frequency-bin to polarization modes, with which our source can be more versatile for various quantum applications. Our scheme can be extended to direct generation of high-dimensional frequency-bin entanglement, and thus will be a key technology for frequency-multiplexed optical quantum information processing.

Time-frequency duality plays a pivotal role in modern optical science and engineering. Conventional duality, which is connected by one-dimensional Fourier transformation, is insufficient for characterizing quantum mechanical correlations in the time-frequency behavior of multiple photons; a higher-dimensional treatment is required. The authors directly measure the two-photon distributions of generated biphotons in both frequency and time domains, and show that they satisfy the Fourier-limited condition in two-dimensional time and frequency space, but not in conventional one-dimensional space. This study helps to pave the way to tomorrow's quantum optical technologies.

The difference and sum-frequency distribution of the biphoton wavefunctions were extracted by applying a Fourier transform on the time-domain Hong-Ou-Mandel interference (HOMI) and the NOON state interference (NOONI) patterns.

In this work, we experimentally manipulate the spectrum and phase of a biphoton wave packet in a two-dimensional frequency space. The spectrum is shaped by adjusting the temperature of the crystal, and the phase is controlled by tilting the dispersive glass plate. The manipulating effects are confirmed by measuring the two-photon spectral intensity (TSI) and the Hong-Ou-Mandel (HOM) interference patterns. Unlike the previous independent manipulation schemes, here we perform joint manipulation on the biphoton spectrum. The technique in this work paves the way for arbitrary shaping of a multi-photon wave packet in a quantum manner., Comment: 4 pages, 4 figures

We investigate the detection of a single-photon source using highly efficient superconducting nanowire single-photon detectors (SNSPDs) at telecom wavelengths. Both the single-photon source and the detectors are characterized in detail. At a pump power of 100 mW (400 mW), the measured coincidence counts can achieve 400 kcps (1.17 Mcps), which is the highest ever reported at telecom wavelengths to the best of our knowledge. The multi-pair contributions, the experimental and theoretical second order coherence functions, and the saturation property of SNSPD are analyzed in detail. The experimental data and theoretical analysis should be useful for the future experiments to detect ultra-bright down-conversion sources with high-efficiency detectors.

Multiparticle interference is a fundamental phenomenon in the study of quantum mechanics.It was discovered in a recent experiment [Ra, Y.-S. et al, Proc. Natl Acad. Sci. USA \textbf{110}, 1227(2013)] that spectrally uncorrelated biphotons exhibited a nonmonotonic quantum-to-classical transition in a four-photon Hong-Ou-Mandel (HOM) interference. In this work, we consider the same scheme with spectrally correlated photons.By theoretical calculation and numerical simulation, we found the transition not only can be nonmonotonic with negative-correlated or uncorrelated biphotons, but also can be monotonic with positive-correlated biphotons. The fundamental reason for this difference is that the HOM-type multi-photon interference is a differential-frequency interference. Our study may shed new light on understanding the role of frequency entanglement in multi-photon behavior., Comment: 8 pages, 2 figures

The NOON state, and its experimental approximation the Holland-Burnett state, have important applications in phase sensing measurement with enhanced sensitivity. However, most of the previous Holland-Burnett state interference (HBSI) experiments only investigated the area of the interference pattern in the region immediately around zero optical path length difference, while the full HBSI pattern over a wide range of optical path length differences has not yet been well explored. In this work, we experimentally and theoretically demonstrate up to six-photon HBSI and study the properties of the interference patterns over a wide range of optical path length differences. It was found that the shape, the coherence time and the visibility of the interference patterns were strongly dependent on the detection schemes. This work paves the way for applications which are based on the envelope of the HBSI pattern, such as quantum spectroscopy and quantum metrology.

Hong-Ou-Mandel (HOM) interference between independent photon sources (HOMI-IPS) is the fundamental block for quantum information processing, such as quantum gate, Shor's algorithm, Boson sampling, etc. All the previous HOMI-IPS experiments were carried out in time-domain, however, the spectral information during the interference was lost, due to technical difficulties. Here, we investigate the HOMI-IPS in spectral domain using the recently developed fast fiber spectrometer, and demonstrate the spectral distribution during the HOM interference between two heralded single-photon sources, and two thermal sources. This experiment can not only deepen our understanding of HOMI-IPS in the spectral domain, but also be utilized to improve the visibility by post-processing spectral filtering., Comment: 8 pages, 7 figures

The classical Wiener-Khinchin theorem (WKT), which can extract spectral information by classical interferometers through Fourier transform, is a fundamental theorem used in many disciplines. However, there is still need for a quantum version of WKT, which could connect correlated biphoton spectral information by quantum interferometers. Here, we extend the classical WKT to its quantum counterpart, i.e., extended WKT (e-WKT), which is based on two-photon quantum interferometry. According to the e-WKT, the difference-frequency distribution of the biphoton wavefunctions can be extracted by applying a Fourier transform on the time-domain Hong-Ou-Mandel interference (HOMI) patterns, while the sum-frequency distribution can be extracted by applying a Fourier transform on the time-domain NOON state interference (NOONI) patterns. We also experimentally verified the WKT and e-WKT in a Mach-Zehnder interference (MZI), a HOMI and a NOONI. This theorem can be directly applied to quantum spectroscopy, where the spectral correlation information of biphotons can be obtained from time-domain quantum interferences by Fourier transform. This may open a new pathway for the study of light-matter interaction at the single photon level., 13 pages, 5 figures

Optical fibres have proved to be an important medium for manipulating and generating light in applications including soliton transmission1, light amplification2, all-optical switching3 and supercontinuum generation4. In the quantum regime, fibres may prove useful for ultralow-power all-optical signal processing5 and quantum information processing6. Here, we demonstrate the first experimental observation of optical nonlinearity at the single-photon level in an optical fibre. Taking advantage of the large nonlinearity and managed dispersion of photonic crystal fibres7,8, we report very small (1 × 10−7 to ∼1 × 10−8 rad) conditional phase shifts induced by weak coherent pulses that contain one or less than one photon per pulse on average. We discuss the feasibility of quantum information processing using optical fibres, taking into account the observed Kerr nonlinearity, accompanied by ultrafast response time and low induced loss. The tiny phase changes introduced by nonlinear optics performed at the single-photon level is reported in a photonic crystal fibre with carefully designed nonlinear and dispersion properties. The approach may prove useful in future quantum information processing schemes.

Entanglement swapping at telecom wavelengths is at the heart of quantum networking in optical fiber infrastructures. Although entanglement swapping has been demonstrated experimentally so far using various types of entangled photon sources both in near-infrared and telecom wavelength regions, the rate of swapping operation has been too low to be applied to practical quantum protocols, due to limited efficiency of entangled photon sources and photon detectors. Here we demonstrate drastic improvement of the efficiency at telecom wavelength by using two ultra-bright entangled photon sources and four highly efficient superconducting nanowire single photon detectors.We have attained a four-fold coincidence count rate of 108 counts per second, which is three orders higher than the previous experiments at telecom wavelengths. A raw (net) visibility in a Hong-Ou-Mandel interference between the two independent entangled sources was 73.3 $\pm$ 1.0% (85.1 $\pm$ 0.8%). We performed the teleportation and entanglement swapping, and obtained a fidelity of 76.3% in the swapping test.Our results on the coincidence count rates are comparable with the ones ever recorded in teleportation/swaping and multi-photon entanglement generation experiments at around 800\,nm wavelengths. Our setup opens the way to practical implementation of device-independent quantum key distribution and its distance extension by the entanglement swapping as well as multi-photon entangled state generation in telecom band infrastructures with both space and fiber links., Comment: 9 pages, 5 figures

We demonstrate a down-conversion-based twin photon source pumped by a 10 GHz repetition-rate-tunable comb laser at 1553 nm wavelength. We show high Hong-Ou-Mandel interference visibilities, which are free from the pump-power induced degradation.

We present two-photon diffraction and interference experiments utilizing parametric down-converted photon pairs (biphotons) and a transmission grating. The biphoton exhibits a diffraction-interference pattern equivalent to an effective single particle with half wavelength of the constituent photons.

Efficient generation and detection of indistinguishable twin photons are at the core of quantum information and communications technology (Q-ICT). These photons are conventionally generated by spontaneous parametric down conversion (SPDC), which is a probabilistic process and hence occurs at a limited rate, which restricts wider applications of Q-ICT. To increase the rate, one had to excite SPDC by higher pump power, while it inevitably produced more unwanted multi-photon components, harmfully degrading quantum interference visibility. Here we solve this problem by using recently developed 10 GHz repetition-rate-tunable comb laser, combined with a group-velocity-matched nonlinear crystal and superconducting nanowire single photon detectors. They operate at telecom wavelengths more efficiently with less noises than conventional schemes, those typically operate at visible and near infrared wavelengths generated by a 76 MHz Ti Sapphire laser and detected by Si detectors. We could show high interference visibilities, which are free from the pump-power induced degradation. Our laser, nonlinear crystal and detectors constitute a powerful tool box, which will pave a way to implementing quantum photonics circuits with variety of good and low-cost telecom components and will eventually realize scalable Q-ICT in optical infra-structures.

We demonstrate pulsed polarization-entangled photons generated from a periodically poled $\mathrm{KTiOPO_4}$ (PPKTP) crystal in a Sagnac interferometer configuration at telecom wavelength. Since the group-velocity-matching (GVM) condition is satisfied, the intrinsic spectral purity of the photons is much higher than in the previous scheme at around 800 nm wavelength. The combination of a Sagnac interferometer and the GVM-PPKTP crystal makes our entangled source compact, stable, highly entangled, spectrally pure and ultra-bright. The photons were detected by two superconducting nanowire single photon detectors (SNSPDs) with detection efficiencies of 70% and 68% at dark counts of less than 1 kcps. We achieved fidelities of 0.981 $\pm$ 0.0002 for $\left| {\psi ^ -} \right\rangle$ and 0.980 $\pm$ 0.001 for $\left| {\psi ^ +} \right\rangle$ respectively. This GVM-PPKTP-Sagnac scheme is directly applicable to quantum communication experiments at telecom wavelength, especially in free space., Comment: 5 pages, 5 figures http://dx.doi.org/10.1364/OE.22.011498

We report on the experimental generation of an entangled state with a spectrally pure heralded single-photon state and a weak coherent state. By choosing group-velocity matching in the nonlinear crystal, our system for producing entangled photons was 60 times brighter than that in the earlier experiment [Phys. Rev. Lett. 90, 240401 (2003)], with no need of bandpass filters. This entanglement system is useful for quantum information protocols that require indistinguishable photons from independent sources., Comment: 7 pages, 5 figures

We demonstrate a Hong-Ou-Mandel interference between two independent, intrinsically pure, heralded single photons from spontaneous parametric down-conversion (SPDC) at telecommunication wavelength. A visibility of $85.5\ifmmode\pm\else\textpm\fi{}8.3%$ was achieved without using any bandpass filter. Thanks to the group-velocity-matched SPDC and superconducting nanowire single-photon detectors (SNSPDs), the fourfold coincidence counts are one order higher than that in the previous experiments. The combination of bright single-photon sources and SNSPDs is a crucial step for future practical quantum infocommunication systems at telecommunication wavelength.

Photon source is one of the fundamental bricks for quantum information and computation systems. A widely-tunable, highly efficient and spectrally pure photon source would be very useful for such applications. In this paper, we present such a source based on spontaneous parametric down conversion (SPDC) in a periodically poled KTiOPO4 (PPKTP) crystal.

We proposed and demonstrated a simple but deterministic scheme for generating polarization-entangled photon pairs at telecommunication wavelengths with type-II quasi-phase-matched spontaneous parametric down-conversion (QPM-SPDC) having two poling periods. We fabricated a LiNbO3 crystal having two poling periods so as to generate entangled photons at two wavelengths, i.e., 1506 nm and 1594 nm. We characterized the two-photon polarization state with state tomography and confirmed that the state was highly entangled.

We report the efficient generation of a four-qubit bound entangled Smolin state. We also demonstrate the activation of the bound entanglement; we make the bound entanglement in the Smolin state distillable with the help of an additional Bell pair.

We report the experimental realization of the four-partite bound-entangled state, i.e., Smolin state [1] and demonstrate the ‘superactivation’ of the bound entanglement. Bound entanglement is a class of multipartite entanglement that cannot be distilled into pure entanglement under local operations and classical communication (LOCC). Despite its undistillable property, this class of entanglement has interesting properties that are expected to be useful in quantum information processing (QIP). For instance, in the Smolin state, the bound entanglement can be activated into distillable entanglement when two of the parties get together. The process is called “unlocking” [1], and has been demonstrated experimentally [2]. More importantly, the bound entanglement can be activated with the help of entanglement in other systems [3]. The activation of bound entanglement, i.e., superactivation, plays an essential role in the QIP protocols using bound entangled states (e.g., remote information concentration [4]).

The reduction of de Broglie wavelength is one of the fascinating characteristics of multiphoton quantum interference. It will be applicable to, for instance, super-resolution imaging beyond the classical diffraction limit and ultrasensitive phase measurement beyond the standard quantum limit. Thus far, the reduced de Broglie wavelength has been experimentally demonstrated using visible or near infrared photons [1–3]. However, it is still a challenging task to demonstrate multiphoton quantum interference in a telecom-wavelength region, because of insufficient quantum efficiencies of single-photon detectors working at telecom wavelength. Also, efficient photon sources of multiple photons that are mutually indistinguishable are essential to carry out various experiments including multiphoton quantum interference and quantum information protocols. In this context, we have developed an efficient photon-pair source designed for such multiphoton experiments at telecom wavelength. Making use of this source, we demonstrate the first measurement of reduced de Broglie wavelength of the four-photon state at the telecom wavelength.

We present an experiment of nonclassical interference between an intrinsically pure heralded single-photon state and a weak coherent state. Our experiment demonstrates that, without the use of bandpass filters, spectrally pure single photons can have high-visibility ($89.4\ifmmode\pm\else\textpm\fi{}0.5%$) interference with photons from a weak coherent field. Our scheme lays the groundwork for future experiments requiring quantum interference between photons in nonclassical states and those in coherent states.

We report the experimental demonstration of four-photon quantum interference using telecom-wavelength photons. Realization of multi-photon quantum interference is essential to linear optics quantum information processing and measurement-based quantum computing. We have developed a source that efficiently emits photon pairs in a pure spectrotemporal mode at a telecom wavelength region, and have demonstrated the quantum interference exhibiting the reduced fringe intervals that correspond to the reduced de Broglie wavelength of up to the four photon `NOON' state. Our result should open a path to practical quantum information processing using telecom-wavelength photons., Comment: 4 pages, 4 figures

We report the generation of pure single‐photon state in the process of spontaneous parametric down‐conversion with extended phase‐matching condition. The measured joint spectral distribution of the photon pairs shows a high purity of the state we prepared. A visibility of 89.4± 0.5% was achieved without any spectral filtering in a nonclassical Hong‐Ou‐Mandel interference between pure heralded single photons and weak coherent photons.

We report broadband entangled photon sources that have control capability of the frequency entanglement. Directly observing the frequency correlation between the constituent photons, we demonstrate the biphoton sources consisting of frequency-correlated or frequency-anticorrelated photons.

We propose a novel scheme to generate polarization entanglement from spatially-correlated photon pairs. We experimentally realized a scheme by means of a spatial correlation effect in a spontaneous parametric down-conversion and a modified Michelson interferometer. The scheme we propose in this paper can be interpreted as a conversion process from spatial correlation to polarization entanglement., 4 pages, 4 figures

We have developed a high-efficiency source of cross-polarized photon pairs in a 800-nm band via type-II quasi-phase matched spontaneous parametric down-conversion using periodically poled lithium niobate. We obtained 25,000 coincidence counts sec-1 mW-1 of the photon pairs.

The purpose of our study is to establish the technique to measure such weak cross-Kerr nonlinearity induced by a single photon in solid states. The experimental set-up is based on a pump-probe measurement.

We propose and demonstrate a novel scheme to generate a polarization entangled state utilizing a spatial correlation effect in parametric down-conversion. We also demonstrate the violation of Bell's inequality.

Characterization of small nonlinear phase shifts will be a key to the optical quantum information processing. We propose and demonstrate a novel technique to measure the nonlinear phase shifts in a waveguide-type Kerr medium.

We have investigated the polarization entanglement between photon pairs generated from a biexciton in a CuCl single crystal via resonant hyper parametric scattering. The pulses of a high repetition pump are seen to provide improved statistical accuracy and the ability to test Bell's inequality. Our results clearly violate the inequality and thus manifest the quantum entanglement and nonlocality of the photon pairs. We also analyzed the quantum state of our photon pairs using quantum state tomography., 4 pages, 5 figures

We present one- and two-photon diffraction and interference experiments involving parametric down-converted photon pairs. By controlling the divergence of the pump beam in parametric down-conversion, the diffraction-interference pattern produced by an object changes from a quantum (perfectly correlated) case to a classical (uncorrelated) one. The observed diffraction and interference patterns are accurately reproduced by Fourier-optical analysis taking into account the quantum spatial correlation. We show that the relation between the spatial correlation and the object size plays a crucial role in the formation of both one- and two-photon diffraction-interference patterns., 10 pages, 13 figures, rev.2

The paper reports the most recent experimental result that exhibits a higher degree of entanglement. They used vapor-phase-grown thin single crystal of CuCl. Since CuCl has a large bandgap (/spl sim/3.4 eV), it is suitable to generate photon pairs in the short wavelength region near ultraviolet.

We demonstrate the entangled photon pair generation via biexciton-resonant hyper parametric scattering in CuCl crystal. Quantum tomographic analysis of the polarization correlation measurements showed that the generated photon pairs had a high degree of polarization entanglement, in consequence of J=0 angular momentum of the biexciton state.

Entanglement is one of the key features of quantum information and communications technology. The method that has been used most frequently to generate highly entangled pairs of photons1,2 is parametric down-conversion. Short-wavelength entangled photons are desirable for generating further entanglement between three or four photons, but it is difficult to use parametric down-conversion to generate suitably energetic entangled photon pairs. One method that is expected to be applicable for the generation of such photons3 is resonant hyper-parametric scattering (RHPS): a pair of entangled photons is generated in a semiconductor via an electronically resonant third-order nonlinear optical process. Semiconductor-based sources of entangled photons would also be advantageous for practical quantum technologies, but attempts to generate entangled photons in semiconductors have not yet been successful4,5. Here we report experimental evidence for the generation of ultraviolet entangled photon pairs by means of biexciton resonant RHPS in a single crystal of the semiconductor CuCl. We anticipate that our results will open the way to the generation of entangled photons by current injection, analogous to current-driven single photon sources6,7.

Diffraction-interference patterns of parametric down-converted photons through a transmission grating by both one- and two-photon detection schemes are presented. The measured patterns are explained by the Fourier analysis of the two-photon wave packet, considering the quantum spatial correlation between the constituent photons. Spatial diffraction-interference patterns were recorded by a two-photon detector consisting of two avalanche photodiodes. For comparison, diffraction-interference patterns of Ti:sapphire laser are also observed using the same apparatus (a uncorrelated case).