arXiv subjects

Ryosuke Shimizu

Publications and source records attributed to Ryosuke Shimizu.

At least 37 records · Page 2Linked to original sources

arXiv2023

Spatial-spectral mapping to prepare the frequency entangled qudits

Entangled qudits, the high-dimensional entangled states, play an important role in the study of quantum information. How to prepare entangled qudits in an efficient and easy-to-operate manner is still a challenge in quantum technology. Here, we demonstrate a method to engineer frequency entangled qudits in a spontaneous parametric downconversion process. The proposal employs an angle-dependent phase-matching condition in a nonlinear crystal, which forms a classical-quantum mapping between the spatial (pump) and spectral (biphotons) degrees of freedom. In particular, the pump profile is separated into several bins in the spatial domain, and thus shapes the down-converted biphotons into discrete frequency modes in the joint spectral space. Our approach provides a feasible and efficient method to prepare a high-dimensional frequency entangled state. As an experimental demonstration, we generate a three-dimensional entangled state by using a homemade variable slit mask.

quant-ph↗

arXiv2023

Freestanding LiPON: from Fundamental Study to Uniformly Dense Li Metal Deposition Under Zero External Pressure

Lithium phosphorus oxynitride (LiPON) is a well-known amorphous thin film solid electrolyte that has been extensively studied in the last three decades. Despite the promises to pair with Li metal anode and various cathode materials, the presence of rigid substrate and LiPONs unique amorphous, air-sensitive nature set limitations to comprehensively understand its intrinsic properties for future development and applications. This work demonstrates a methodology to synthesize LiPON in a freestanding form that exhibits remarkable flexibility and a Young s modulus of ~33 GPa. Solid-state nuclear magnetic resonance (ss-NMR) and differential scanning calorimetry (DSC) results with unprecedented high signal-to-noise ratio could be obtained with such freestanding LiPON (FS-LiPON), revealing the Li-LiPON interface bonding environments quantitatively and a well-defined glass transition temperature for LiPON. Combining interfacial stress and a seeding layer, FS-LiPON demonstrates a uniform and fully dense Li metal deposition without the aid of external pressure. Such a FS-LiPON film offers new opportunities for fundamental study of LiPON material and associated interfaces, and provides perspectives for interface engineering in bulk solid-state battery.

cond-mat.mtrl-sci↗

arXiv2023

Construction of $p$-energy and associated energy measures on Sierpiński carpets

We establish the existence of a scaling limit $\mathcal{E}_p$ of discrete $p$-energies on the graphs approximating generalized Sierpiński carpets for $p > \dim_{\text{ARC}}(\textsf{SC})$, where $\dim_{\text{ARC}}(\textsf{SC})$ is the Ahlfors regular conformal dimension of the underlying generalized Sierpiński carpet. Furthermore, the function space $\mathcal{F}_{p}$ defined as the collection of functions with finite $p$-energies is shown to be a reflexive and separable Banach space that is dense in the set of continuous functions with respect to the supremum norm. In particular, $(\mathcal{E}_2, \mathcal{F}_2)$ recovers the canonical regular Dirichlet form constructed by Barlow and Bass or Kusuoka and Zhou. We also provide $\mathcal{E}_{p}$-energy measures associated with the constructed $p$-energy and investigate its basic properties like self-similarity and chain rule.

math.MG↗

arXiv2022

Unraveling the stable cathode electrolyte interface in all solid-state thin-film battery operating at 5V

Spinel-type LiNi0.5Mn1.5O4 (LNMO) is one of the most promising 5 V-class cathode materials for Li-ion batteries that can achieve high energy density and low production costs. However, in liquid electrolyte cells, the high voltage causes continuous cell degradation through the oxidative decomposition of carbonate-based liquid electrolytes. In contrast, some solid-state electrolytes have a wide electrochemical stability range and can withstand the required oxidative potential. In this work, a thin-film battery consisting of a LNMO cathode with a solid lithium phosphorus oxynitride (LiPON) electrolyte is tested and their interface before and after cycling is characterized. With Li metal as the anode, this system can deliver stable performance for 600 cycles with an average Coulombic efficiency > 99%. Neutron depth profiling indicates a slight overlithiated layer at the interface prior to cycling; a result that is consistent with the excess charge capacity measured during the first cycle. Cryogenic electron microscopy further reveals intimate contact between LNMO and LiPON without noticeable structure and chemical composition evolution after extended cycling, demonstrating the superior stability of LiPON against a high voltage cathode. Consequently, we propose design guidelines for interface engineering that could accelerate the commercialization of a high voltage cell with solid or liquid electrolytes.

cond-mat.mtrl-sci↗

arXiv2021

Quantum Fourier transform spectroscopy of biexciton

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. Here, we report the first experimental demonstration of two-photon quantum interference of photon pairs emitted via biexcitons in the semiconductor CuCl. Besides applying Fourier transform to quantum interference patterns, we reconstruct the intensity spectrum of the biexciton luminescence in the two-photon sum or difference frequency. We discuss the connection between the reconstructed spectra and exciton states in CuCl as well as the capability of quantum interferometry in solid-state spectroscopy.

quant-ph↗

arXiv2021

Broadband-laser-diode pumped PPKTP-Sagnac polarization-entangled photon source

We experimentally demonstrate a polarization-entangled photon source at 810 nm using a type-II phase-matched 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 nm and 7.32 nm. We prepare two Bell states |Psi+> and |Psi-> with the fidelities of 0.948+-0.004 and 0.963+-0.002. In 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. To our knowledge, this experiment is the first to combine a multi-mode pump laser with a Sagnac-loop configuration. This high-quality and low-cost entangled photon source may have many practical applications in quantum information processing.

quant-ph↗

arXiv2021

Spectrally resolved NOON state interference

NOON state interference (NOON-SI) is a powerful tool to improve the phase sensing precision, and plays an important role in quantum measurement. In most of the previous NOON-SI experiments, the measurements were performed in time domain where the spectral information of the involved photons was integrated and lost during the measurement. In this work, we experimentally measured the joint spectral intensities (JSIs) at different positions of the interference patterns in both time and frequency domains. It was observed that the JSIs were phase-dependent and show odd (even)-number patterns at $0$ ($π$) phase shift; while no interference appeared in time domain measurement, the interference pattern clearly appeared in frequency domain. To our best knowledge, the latter is the first observation of the spectrally resolved NOON state interference, which provides alternative information that cannot be extracted from the time-domain measurement. To explore its potential applications, we considered the interferometric sensing with our setup. From the Fisher information-based analysis, we show that the spectrally resolved NOON-SI has a better performance at non-zero-delay position than its non-spectrally resolved counterpart. The spectrally resolved NOON-SI scheme may be useful for quantum metrology applications such as quantum phase sensing, quantum spectroscopy, and remote synchronization.

quant-ph↗

arXiv2020

Mid-infrared spectrally-uncorrelated biphotons generation from doped PPLN: a theoretical investigation

We theoretically investigate the preparation of mid-infrared (MIR) spectrally-uncorrelated biphotons from a spontaneous parametric down-conversion process using doped LN crystals, including MgO doped LN, ZnO doped LN, and In2O3 doped ZnLN with doping ratio from 0 to 7 mol%. The tilt angle of the phase-matching function and the corresponding poling period are calculated under type-II, type-I, and type-0 phase-matching conditions. We also calculate the thermal properties of the doped LN crystals and their performance in Hong-Ou-Mandel interference. It is found that the doping ratio has a substantial impact on the group-velocity-matching (GVM) wavelengths. Especially, the GVM2 wavelength of co-doped InZnLN crystal has a tunable range of 678.7 nm, which is much broader than the tunable range of less than 100 nm achieved by the conventional method of adjusting the temperature. It can be concluded that the doping ratio can be utilized as a degree of freedom to manipulate the biphoton state. The spectrally uncorrelated biphotons can be used to prepare pure single-photon source and entangled photon source, which may have promising applications for quantum-enhanced sensing, imaging, and communications at the MIR range.

quant-ph↗

arXiv2020

Unveiling the Stable Nature of the Solid Electrolyte Interphase between Lithium Metal and LiPON via Cryogenic Electron Microscopy

The solid electrolyte interphase (SEI) is regarded as the most complex but the least understood constituent in secondary batteries using liquid and solid electrolytes. The nanostructures of SEIs were recently reported to be equally important to the chemistry of SEIs for stabilizing Li metal in liquid electrolyte. However, the dearth of such knowledge in all-solid-state battery (ASSB) has hindered a complete understanding of how certain solid-state electrolytes, such as LiPON, manifest exemplary stability against Li metal. Characterizing such solid-solid interfaces is difficult due to the buried, highly reactive, and beam-sensitive nature of the constituents within. By employing cryogenic electron microscopy (cryo-EM), the interphase between Li metal and LiPON is successfully preserved and probed, revealing a multilayer mosaic SEI structure with concentration gradients of nitrogen and phosphorous, materializing as crystallites within an amorphous matrix. This unique SEI nanostructure is less than 80 nm and is shown stable and free of any organic lithium containing species or lithium fluoride components, in contrast to SEIs often found in state-of-the-art organic liquid electrolytes. Our findings reveal insights on the nanostructures and chemistry of such SEIs as a key component in lithium metal batteries to stabilize Li metal anode.

cond-mat.mtrl-sci↗

arXiv2020

Local structure of glassy lithium phosphorus oxynitride thin films: a combined experimental and ab initio approach

Lithium phosphorus oxynitride (LiPON) is an amorphous solid-state lithium ion conductor displaying exemplary cyclability against lithium metal anodes. There is no definitive explanation for this stability due to the limited understanding of the structure of LiPON. We provide a structural model of RF-sputtered LiPON via experimental and computational spectroscopic methods. Information about the short-range structure results from 1D and 2D solid-state nuclear magnetic resonance experiments investigating chemical shift anisotropy and dipolar interactions. These results are compared with first principles chemical shielding calculations of Li-P-O/N crystals and ab initio molecular dynamics-generated amorphous LiPON models to unequivocally identify the glassy structure as primarily isolated phosphate monomers with N incorporated in both apical and as bridging sites in phosphate dimers. Structural results suggest LiPON's stability is a result of its glassy character. Free-standing LiPON films are produced that exhibit a high degree of flexibility highlighting the unique mechanical properties of glassy materials.

cond-mat.mtrl-sci↗

arXiv2020

Generation of pseudo-sunlight via quantum entangled photons and the interaction with molecules

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.

quant-ph↗

arXiv2020

Quantum optical synthesis in 2D time-frequency space

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.

quant-ph↗

arXiv2019

Spectrally uncorrelated biphotons generated from `the family of BBO crystal'

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.

quant-ph↗

arXiv2019

Theoretical investigation of a spectrally pure-state generation from isomorphs of KDP crystal at near-infrared and telecom wavelengths

Spectrally uncorrelated biphoton state generated from the spontaneous nonlinear optical process is an important resource for quantum information. Currently such spectrally uncorrelated biphoton state can only be prepared from limited kinds of nonlinear media, thus limiting their wavelengths. In order to explore wider wavelength range, here we theoretically study the generation of spectrally uncorrelated biphoton state from 14 isomorphs of potassium dihydrogen phosphate (KDP) crystal. We find that 11 crystals from the `KDP family' still maintain similar nonlinear optical properties of KDP, such as KDP, DKDP, ADP, DADP, ADA, DADA, RDA, DRDA, RDP, DRDP and KDA, which satisfy 3 kinds of the group-velocity matching conditions for spectrally uncorrelated biphoton state generation from near-infrared to telecom wavelengths. Based on the uncorrelated biphoton state, we investigate the generation of heralded pure-state single photon by detecting one member of the biphoton state to herald the output of the other. The purity of the heralded single photon is as high as 0.98 without using a narrow-band filter; the Hong-Ou-Mandel interference from independent sources can also achieve a visibility of 98%. This study may provide more and better single-photon sources for quantum information processing at near-infrared and telecom wavelengths.

quant-ph↗

arXiv2018

Direct generation of frequency-bin entangled photons via two-period quasi-phase-matched parametric downconversion

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.

quant-ph↗

arXiv2018

Quantum manipulation of biphoton spectral distributions in a 2D frequency space toward arbitrary shaping of a biphoton wave packet

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.

quant-ph↗

arXiv2018

Experimental demonstration of time-frequency duality of biphotons

Time-frequency duality, which enables control of optical waveforms by manipulating amplitudes and phases of electromagnetic fields, plays a pivotal role in a wide range of modern optics. The conventional one-dimensional (1D) time-frequency duality has been successfully applied to characterize the behavior of classical light, such as ultrafast optical pulses from a laser. However, the 1D treatment is not enough to characterize quantum mechanical correlations in the time-frequency behavior of multiple photons, such as the biphotons from parametric down conversion. The two-dimensional treatment is essentially required, but has not been fully demonstrated yet due to the technical problem. Here, we study the two-dimensional (2D) time-frequency duality duality of biphotons, by measuring two-photon distributions in both frequency and time domains. It was found that generated biphotons satisfy the Fourier limited condition quantum mechanically, but not classically, by analyzing the time-bandwidth products in the 2D Fourier transform. Our study provides an essential and deeper understanding of light beyond classical wave optics, and opens up new possibilities for optical synthesis in a high-dimensional frequency space in a quantum manner.

quant-ph↗

arXiv2017

Extended Wiener-Khinchin theorem for quantum spectral analysis

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.

quant-ph↗