Coherence Lifetime Research Articles

Phase separation in alkali silicate glasses detected through inverse Laplace transform of29Si nuclear magnetic resonance echo train decay

The ratio of Si-29 nuclear magnetic resonance coherence lifetimes for Q4and Q3sites under magic-angle spinning and a π-pulse train in silicate glasses can detect phase separation, even at small scales where the glass appears optically homogenous.

Effects of Microwave Gating on Nuclear Spin Echoes in Dynamic Nuclear Polarization.

Dipolar or quadrupolar echoes allow one to observe undistorted powder patterns, in contrast to simple Fourier transformations of free induction decays (FIDs). In this work, the buildup of proton polarization due to dynamic nuclear polarization (DNP) is monitored by observing echoes rather than FIDs. When the microwave irradiation is interrupted during the buildup of DNP, the electrons relax back to their Boltzmann distribution at high fields (B0 = 6.7 T) and low temperatures 1.2 < Tsample < 4.0 K, so that dipolar flip-flop-flip terms involving two electrons and one proton become largely ineffective as a mechanism of proton decoherence. This leads to a prolongation of the nuclear coherence lifetime T2'(1H). The increase in T2'(1H) leads to transient surges of the amplitudes of spin echoes. Conversely, transient slumps of spin echoes are observed when the microwave irradiation is switched back on, due to a shortening of nuclear coherence lifetimes.

Photoredox-Mediated Sensitization of Lanthanide Dopants by Perovskite Nanocrystals

Trivalent lanthanide ions (Ln3+) have electronically isolated f-orbitals that support excited states, which, due to their ultra-narrow emission and long spin coherence lifetimes, are potentially suitable as hosts for spin qubits. These excited states must however be generated through photosensitization due to the low-absorption cross sections of Ln3+. This paper describes the mechanism of photosensitization of Yb3+ and Sm3+ ions by their CsPbCl3 perovskite nanocrystal (NC) host matrices, through examination of the photophysical processes in NCs doped with seven different Ln3+ ions. An observed dependence of the NC’s band-edge photoluminescence (PL) on the potential of the Ln3+/Ln2+ redox couple implies the presence of a charge transfer intermediate in the sensitization mechanism. Ultrafast transient absorption (TA) experiments indicate that (i) a previously identified Ln3+-Cl–-VPb2–-Cl–-Ln3+ defect is formed within 1 ps of photoexcitation of the NC regardless of the yield of photosensitization, (ii) the first step of photosensitization, an electron transfer, occurs in 10s of picoseconds, and (iii) the resulting charge-separated state forms the emissive species, Ln3+*, through a slower subsequent hole transfer from the NC. A mechanistic understanding of Ln3+ dopant sensitization provides a framework for choosing the right combination of host matrix and Ln3+ species for efficient photosensitization.

Silicon-29 echo train coherence lifetimes and geminal [formula omitted]-couplings in network modified silicate glasses

The natural abundance 29Si echo-train coherence lifetimes in network-modified silicate glasses were examined under static and magic-angle spinning (MAS) conditions. The nuclear magnetic properties of modifier cations were found to play a major role in determining 29Si coherence lifetimes, leading to differences as large as three orders of magnitude. In compositions with abundant NMR active nuclei, such as alkali silicates, the 29Si coherence lifetimes are dominated by coherent dephasing due to residual heteronuclear dipolar couplings, whereas in compositions dilute in NMR active nuclei, such as alkaline earth silicates, the 29Si coherence lifetimes are dominated by incoherent dephasing due to paramagnetic impurities. Expressing the inverse of the coherence lifetime as a residual full width at half maximum (FWHM), we found that increasing rates of both MAS and a π-pulse train are effective in removing the residual 29Si heteronuclear broadenings, with a near-linear relationship between FWHM and MAS rotor period and π-pulse spacing. Based on these results, we conclude that accurate 29Si J coupling measurements will be the most challenging in lithium silicate glasses due to strong homonuclear dipolar couplings among 7Li nuclei, requiring MAS speeds up to 100 kHz, and be the least challenging in the alkaline earth silicate glasses. At a modest MAS speed of 14kHz, distributions of geminal J couplings across Si-O-Si linkages were measured in alkali and alkaline earth silicate glasses giving mean values of 4.2Hz and 5.1Hz in 0.4 CaO·0.6 SiO2 and 0.33 Ba2O·0.67 SiO2 glasses, respectively, and 5.2Hz and 5.3Hz in 0.33 Na2O·0.67 SiO2 and 0.33 K2O·0.67 SiO2 glasses, respectively. We also observe greater variance in the J distributions of alkaline earth silicate glasses consistent with greater structural disorder due to increased modifier cation potential, i.e., the charge-to-radius ratio, Z/r of the cation.

Coupled valence carrier and core-exciton dynamics in WS2 probed by few-femtosecond extreme ultraviolet transient absorption spectroscopy

Few-femtosecond extreme ultraviolet (XUV) transient absorption spectroscopy, performed with optical 500-1000 nm supercontinuum and broadband XUV pulses (30-50 eV), simultaneously probes dynamics of photoexcited carriers in WS$_{2}$ at the W O$_3$ edge (37-45 eV) and carrier-induced modifications of core-exciton absorption at the W N$_{6,7}$ edge (32-37 eV). Access to continuous core-to-conduction band absorption features and discrete core-exciton transitions in the same XUV spectral region in a semiconductor provides a novel means to investigate the effect of carrier excitation on core-exciton dynamics. The core-level transient absorption spectra, measured with either pulse arriving first to explore both core-level and valence carrier dynamics, reveal that core-exciton transitions are strongly influenced by the photoexcited carriers. A $1.2\pm0.3$ ps hole-phonon relaxation time and a $3.1\pm0.4$ ps carrier recombination time are extracted from the XUV transient absorption spectra from the core-to-conduction band transitions at the W O$_{3}$ edge. Global fitting of the transient absorption signal at the W N$_{6,7}$ edge yields $\sim 10$ fs coherence lifetimes of core-exciton states and reveals that the photoexcited carriers, which alter the electronic screening and band filling, are the dominant contributor to the spectral modifications of core-excitons and direct field-induced changes play a minor role. This work provides a first look at the modulations of core-exciton states by photoexcited carriers and advances our understanding of carrier dynamics in metal dichalcogenides.

Spectroscopic Analysis of Vibronic Relaxation Pathways in Molecular Spin Qubit [Ho(W5O18)2]9-: Sparse Spectra Are Key.

Vibrations play a prominent role in magnetic relaxation processes of molecular spin qubits as they couple to spin states, leading to the loss of quantum information. Direct experimental determination of vibronic coupling is crucial to understand and control the spin dynamics of these nano-objects, which represent the limit of miniaturization for quantum devices. Herein, we measure the magneto-infrared properties of the molecular spin qubit system Na9[Ho(W5O18)2]·35H2O. Our results place significant constraints on the pattern of crystal field levels and the vibrational excitations allowing us to unravel vibronic decoherence pathways in this system. We observe field-induced spectral changes near 63 and 370 cm-1 that are modeled in terms of odd-symmetry vibrations mixed with f-manifold crystal field excitations. The overall extent of vibronic coupling in Na9[Ho(W5O18)2]·35H2O is limited by a modest coupling constant (on the order of 0.25) and a transparency window in the phonon density of states that acts to keep the intramolecular vibrations and MJ levels apart. These findings advance the understanding of vibronic coupling in a molecular magnet with atomic clock transitions and suggest strategies for designing molecular spin qubits with improved coherence lifetimes.

Solid state core-exciton dynamics in NaCl observed by tabletop attosecond four-wave mixing spectroscopy

Nonlinear wave mixing in solids with ultrafast x-rays can provide insight into complex electronic dynamics of materials. Here, tabletop-based attosecond noncollinear four-wave mixing (FWM) spectroscopy using one extreme ultraviolet (XUV) pulse from high harmonic generation and two separately timed few-cycle near-infrared (NIR) pulses characterizes the dynamics of the ${\mathrm{Na}}^{+}$ ${L}_{2,3}$ edge core-excitons in NaCl around 33.5 eV. An inhomogeneous distribution of core-excitons underlying the well-known doublet absorption of the ${\mathrm{Na}}^{+}$ $\mathrm{\ensuremath{\Gamma}}$ point core-exciton spectrum is deconvoluted by the resonance-enhanced nonlinear wave mixing spectroscopy. In addition, other dark excitonic states that are coupled to the XUV-allowed levels by the NIR pulses are characterized spectrally and temporally. Approximately $&lt;10\phantom{\rule{0.16em}{0ex}}\mathrm{fs}$ coherence lifetimes of the core-exciton states are observed. The core-excitonic properties are discussed in the context of strong electron-hole exchange interactions, electron-electron correlation, and electron-phonon broadening. This investigation successfully indicates that tabletop attosecond FWM spectroscopies represent a viable technique for time-resolved solid state measurements.

Prediction Based on Type-II Censored Coherent System Lifetime Data under a Proportional Reversed Hazard Rate Model

Prediction Based on Type-II Censored Coherent System Lifetime Data under a Proportional Reversed Hazard Rate Model

Excitation relaxation in a molecular chain and energy transfer at steady state.

We consider the reduced dynamics of a molecular chain weakly coupled to a phonon bath. With a small and constant inhomogeneity in the coupling, the excitation relaxation rates are obtained in closed form. They are dominated by transitions between exciton modes lying next to each other in the energy spectrum. The rates are quadratic in the number of sites in a long chain. Consequently, the evolution of site occupation numbers exhibits longer coherence lifetime for short chains only. When external source and sink are added, the rate equations of exciton occupation numbers are similar to those obtained earlier by Fröhlich to explain energy storage and energy transfer in biological systems. There is a clear separation of timescale into a faster one pertaining to internal influence of the chain and phonon bath, and a slower one determined by external influence, such as the pumping rate of the source, the absorption rate of the sink, and the rate of radiation loss. The energy transfer efficiency at steady state depends strongly on these external parameters and is robust against a change in the internal parameters, such as temperature and inhomogeneity. Excitations are predicted to concentrate to the lowest energy mode when the source power is sufficiently high. In the site basis, this implies that when sustained by a high power source, a sink positioned at the center of the chain is more efficient in trapping energy than a sink placed at its end. Analytic expressions of energy transfer efficiency are obtained in the high power and low-power source limit. Parameters of a photosynthetic system are used as examples to illustrate the results.

Optical spin-state polarization in a binuclear europium complex towards molecule-based coherent light-spin interfaces

The success of the emerging field of solid-state optical quantum information processing (QIP) critically depends on the access to resonant optical materials. Rare-earth ion (REI)-based molecular systems, whose quantum properties could be tuned taking advantage of molecular engineering strategies, are one of the systems actively pursued for the implementation of QIP schemes. Herein, we demonstrate the efficient polarization of ground-state nuclear spins—a fundamental requirement for all-optical spin initialization and addressing—in a binuclear Eu(III) complex, featuring inhomogeneously broadened 5D0 → 7F0 optical transition. At 1.4 K, long-lived spectral holes have been burnt in the transition: homogeneous linewidth (Γh) = 22 ± 1 MHz, which translates as optical coherence lifetime (T2opt) = 14.5 ± 0.7 ns, and ground-state spin population lifetime (T1spin) = 1.6 ± 0.4 s have been obtained. The results presented in this study could be a progressive step towards the realization of molecule-based coherent light-spin QIP interfaces.

Delayed failure under static fatigue of Hi-Nicalon bundles: The role of stress dispersion on scale effect

SiC-fibers are subjected to a predictable premature failure, consequence of a slow crack growth mechanism. This has chiefly been studied through static fatigue testing of multifilament tows. The discrepancy existing between experimental results, broadly dispersed, and the bundle theory (solely considering the filament strength distribution) has been interpreted by discrete stochastic phenomena. In this work, the uncertainty on applied stress caused by fiber misalignment (slack) was rather investigated through Monte Carlo simulation, ascribing to each filament of the tow a strength and a stress among established distributions. If a coherent lifetime range could this way be obtained, a scale effect on stress exponent was also revealed: equal to 12.6 on filament it falls to 8.4 on bundle, in agreement with experimental results. The same would apply to larger scale (woven tow).

Understanding radiative transitions and relaxation pathways in plexcitons

Summary Molecular aggregates on plasmonic nanoparticles have emerged as attractive systems for the studies of polaritonic light-matter states, called plexcitons. Such systems are tunable, scalable, easy to synthesize, and offer sub-wavelength confinement, all while giving access to the ultrastrong light-matter coupling regime, promising a plethora of applications. However, the complexity of these materials prevented the understanding of their excitation and relaxation phenomena. Here, we follow the relaxation pathways in plexcitons and conclude that while the metal destroys the optical coherence, the molecular aggregate coupled to surface processes significantly contributes to the energy dissipation. We use two-dimensional electronic spectroscopy with theoretical modeling to assign the different relaxation processes to either molecules or metal nanoparticle. We show that the dynamics beyond a few femtoseconds has to be considered in the language of hot electron distributions instead of the accepted lower and upper polariton branches and establish the framework for further understanding.

A Magic Angle Spinning Activated 17O DNP Raser.

In the raser effect, a sample spontaneously emits continuous radiofrequency radiation, allowing exceptionally narrow NMR line widths to be recorded without applying pulses. To achieve this phenomenon, a large negative magnetization must be induced, which we show here can be achieved for the 17O magnetization of isotopically labeled Gd-doped CeO2 using solid effect dynamic nuclear polarization (DNP), at high field and 110 K. This allows a 2 mHz line width to be measured, which is limited only by the magnetic field stability. The raser effect can be reversibly activated and deactivated by magic angle spinning (MAS), which modulates the nuclear spin coherence lifetime. The use of MAS DNP to enable the raser effect should be further applicable to other systems and nuclei.

Single-shot fs/ns rotational CARS for temporally and spectrally resolved gas-phase diagnostics

We report thermometry and new Raman linewidth data using a novel method for time-domain rotational coherent anti-Stokes Raman spectroscopy (RCARS) on single-shot basis. The coherences are generated by two fs pulses and probed by a ns pulse. The resulting signal is detected using a combined spectrograph/streak camera setup with high spectral and temporal resolution. Rotational CARS spectrograms of nitrogen (N2), ethylene (C2H4), ethane (C2H6), and argon (Ar) are demonstrated at ambient condition. Self-broadened N2–N2 S-branch Raman linewidths were measured on single-shot basis and show excellent agreement with literature values. Furthermore, Raman linewidths of N2 S-branch perturbed by C2H4 and C2H6 were measured for the first time. The time-resolved approach was also utilized to separate complex spectra from a mixture of species through their difference in coherence lifetimes. Since the Raman coherences decay much faster for both ethane and ethylene than for nitrogen, pure nitrogen spectra could be obtained by analyzing only the temporal tail of the signal. Moreover, a model for time-resolved RCARS of N2 was developed, which employs the single-shot measured Raman linewidths to calculate the corresponding spectro-temporally resolved spectrograms at different temperatures. The model was used to evaluate the temperature from single-shot data of an N2/C2H6 mixture, showing very high accuracy. The demonstrated method constitutes an essential improvement for single-shot thermometry as it does not require pre-knowledge about collider species concentrations and their impact on linewidths.

Silicon-Integrated Telecommunications Photon-Spin Interface

Long-distance entanglement distribution is a vital capability for quantum technologies. An outstanding practical milestone towards this aim is the identification of a suitable matter-photon interface which possesses, simultaneously, long coherence lifetimes and efficient telecommunications-band optical access. In this work, alongside its sister publication, we report upon the T center, a silicon defect with spin-selective optical transitions at 1326 nm in the telecommunications O-band. Here we show that the T center in $^{28}$Si offers electron and nuclear spin lifetimes beyond a millisecond and second respectively, as well as optical lifetimes of 0.94(1) $\mu$s and a Debye-Waller factor of 0.23(1). This work represents a significant step towards coherent photonic interconnects between long-lived silicon spins, spin-entangled telecom single-photon emitters, and spin-dependent silicon-integrated photonic nonlinearities for future global quantum technologies.

A Frequency-Multiplexed Coherent Electro-optic Memory in Rare Earth Doped Nanoparticles.

Quantum memories for light are essential components in quantum technologies like long-distance quantum communication and distributed quantum computing. Recent studies have shown that long optical and spin coherence lifetimes can be observed in rare earth doped nanoparticles, opening exciting possibilities over bulk materials, e.g., for enhancing coupling to light and other quantum systems, and material design. Here, we report on coherent light storage in Eu3+:Y2O3 nanoparticles using the Stark echo modulation memory (SEMM) quantum protocol. We first measure a nearly constant Stark coefficient of 50 kHz/(V/cm) across a bandwidth of 15 GHz, which is promising for broadband operation. Storage of light is then demonstrated with an effective coherence lifetime of 5 μs. Pulses with two different frequencies are also stored, confirming frequency-multiplexing capability, and are used to demonstrate the memory high phase fidelity. These results open the way to nanoscale optical quantum memories with increased efficiency, bandwidth, and processing capabilities.

Trap and isolate to extend quantum lifetime

Quantum Sensing The coherence time of a quantum system is an important parameter in the development of technologies that exploit the sensitive nature of quantum mechanics. Rubidium atoms have quantum mechanical spin, each atom behaving like a tiny magnetic compass, which makes them exquisitely sensitive to local fluctuations in the magnetic field. Upadhyay et al. trapped single rubidium atoms in an ultracold parahydrogen matrix and then applied a sequence of pulses that further decoupled them from their immediate decoherence-inducing environment. With this trap-and-isolate protocol, the coherence lifetime of the rubidium atoms can be extended to a fraction of a second. The authors suggest that co-trapping a single molecule alongside a single rubidium atom could provide a platform for single-molecule nuclear magnetic resonance studies and the development of other quantum sensing technologies. Phys. Rev. Lett. 125 , 043601 (2020).

Chemically vapor deposited Eu3+:Y2O3 thin films as a material platform for quantum technologies

Rare earth ions hosted in solids are good candidates for quantum technologies due to their chemical stability and optical and spin transitions exhibiting long coherence lifetimes. While bulk oxide crystals are usually the preferred host material, the development of a scalable silicon-compatible thin film platform would be desirable. In this paper, we report on the growth of Y2(1−x)Eu2xO3 thin films on silicon in the full range of Eu3+ concentration by direct liquid injection chemical vapor deposition (CVD). Our sub-micrometer polycrystalline films with a strong-(111) texture were grown for all compositions into the bixbyite cubic phase. The variation of growth rates with temperature and flow indicated that deposition occurred through a mass-transport controlled regime. Optical assessment of the Eu-doped thin films showed inhomogeneous linewidths as narrow as 50 GHz and fluorescence lifetimes of 1 ms for the lowest concentrations. Finally, a spectral hole was successfully burned in a 200 nm-thin film with a 2% Eu doping leading to a homogeneous linewidth of 11 MHz. These values are still below those reported for bulk single crystals indicating that additional decoherence mechanisms exist in such nanometric films, which might be alleviated by further improvement of the crystalline quality. Nevertheless, these results pave the way to the use of CVD-grown Eu:Y2O3 thin films as a platform for integrated quantum devices.

Extended cumulative entropy based on kth lower record values for the coherent systems lifetime

Kayal (Probab. Eng. Inf. Sci. 30(4):640–662, 2016) first proposed generalized cumulative entropy based on lower record values. Motivated by Kayal (Probab. Eng. Inf. Sci. 30(4):640–662, 2016), recently, Tahmasebi and Eskandarzadeh (Stat. Probab. Lett. 126:164–172, 2017) proposed an extended cumulative entropy (ECE) based on kth lower record values. In this paper, we obtain some properties of ECE. We study this measure of information for the coherent systems lifetime with identically distributed components. We define the conditional ECE for the system lifetime and discuss some properties of it. We also use this idea to propose a measure of extended cumulative past inaccuracy. Finally, we propose the estimators of these measures using empirical approach. In addition, we study large sample properties of these estimators.

Defect Engineering for Quantum Grade Rare-Earth Nanocrystals.

Nanostructured systems that combine optical and spin transitions offer new functionalities for quantum technologies by providing efficient quantum light-matter interfaces. Rare-earth (RE) ion-doped nanoparticles are promising in this field as they show long-lived optical and spin quantum states. However, further development of their use in highly demanding applications, such as scalable single-ion-based quantum processors, requires controlling defects that currently limit coherence lifetimes. In this work, we show that a post-treatment process that includes multistep high-temperature annealing followed by high-power microwave oxygen plasma processing advantageously improves key properties for quantum technologies. We obtain single crystalline Eu3+:Y2O3 nanoparticles (NPs) of 100 nm diameter, presenting bulk-like inhomogeneous line widths (Γinh) and population lifetimes (T1). Furthermore, a significant coherence lifetime (T2) extension, up to a factor of 5, is successfully achieved by modifying the oxygen-related point defects in the NPs by the oxygen plasma treatment. These promising results confirm the potential of engineered RE NPs to integrate devices such as cavity-based single-photon sources, quantum memories, and processors. In addition, our strategy could be applied to a large variety of oxides to obtain outstanding crystalline quality NPs for a broad range of applications.