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At least 127 records · Page 7

Study of perovskite CsPbBr 3 detector polarization and its mitigation with ultrahigh x-ray flux

High-flux capable semiconductor x-ray detectors are essential in various applications, but the detrimental effects of detector polarization limit their use in many cases. Here, for this work, we studied the polarization of perovskite CsPbBr 3 semiconductor detectors using ultrahigh flux synchrotron x rays (10 6 –10 12 photons s –1 mm –2 at 58.61 keV). The CsPbBr 3 detectors did not show immediate polarization prominently until a flux higher than 10 10 photons s –1 mm –2 . Using the pump-and-probe technique, we visualized the spatial and temporal effects of polarization. The polarized region, represented by reduced photocurrent, extended beyond the area under direct irradiation, and the reduced photocurrent persisted after potential de-polarization treatments. We found that stronger applied electric fields and fewer carrier traps can mitigate polarization, represented by less photocurrent deficit. By examining the detectors’ current response under controlled ambient light, low, and high-flux x rays, we studied the trap filling and release behavior of CsPbBr 3 . We discovered that the polarization is caused by partial detector damage due to deep defects generated by ultrahigh flux x-ray irradiation. Our work provides insight into CsPbBr 3 polarization under extremely intense x-ray radiation and shows that reducing crystal defects and increasing detector bias voltage are effective solutions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Two-tone Doppler cooling of radial two-dimensional crystals in a radio-frequency ion trap

We study the Doppler-cooling of radial two-dimensional (2D) Coulomb crystals of trapped barium ions in a radiofrequency trap. Ions in radial 2D crystals experience micromotion of an amplitude that increases linearly with the distance from the trap center, leading to a position-dependent frequency modulation of laser light in each ion's rest frame. We use two tones of Doppler-cooling laser light separated by approximately 100 MHz to efficiently cool distinct regions in the crystals with differing amplitudes of micromotion. This technique allows us to trap and cool more than 50 ions populating 4 shells in a radial two-dimensional crystal, where with a single tone of Doppler cooling light we are limited to 30 ions in 3 shells. Here, we also individually characterize the micromotion of all ions within the crystals, and use this information to locate the center of the trap and to determine the Matthieu parameters q x and q y .

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Mitigation of J–V distortion in CdTe solar cells by Ga-doping of MgZnO emitter

Distortions in the current–voltage curves of CdTe-based thin-film solar cells with MgZnO emitter layers are not uncommon. Even when such distortions are very subtle with standard sunlight, they can be greatly accentuated by the removal of short-wavelength photons with optical filters, and the dark-curve turn-on voltage can be noticeably increased. The strong suggestion is that good J–V curves with full-spectrum light often rely on photogeneration of electrons from trap states in the MgZnO emitter. When the carrier concentration of the CdTe absorber is increased with external doping, there is a corresponding need for a larger MgZnO carrier concentration. Based on the assumption that the emitter carrier concentration needs to be comparable to that of the absorber, Ga-doping of the MgZnO was shown to very nearly eliminate the large filtered-light distortions and is arguably superior to MgZnO that relies on photogeneration. In addition, it was shown that photogeneration and recovery in MgZnO is relatively slow, so that without Ga-doping, the cell efficiency improves gradually for most of an hour in the light, and the turn-on voltage of the dark curve increases on a similar time scale when the light is removed.

36 MATERIALS SCIENCE↗

High-fidelity trapped-ion qubit operations with scalable photonic modulators

Abstract Experiments with trapped ions and neutral atoms typically employ optical modulators in order to control the phase, frequency, and amplitude of light directed to individual atoms. These elements are expensive, bulky, consume substantial power, and often rely on free-space I/O channels, all of which pose scaling challenges. To support many-ion systems like trapped-ion quantum computers or miniaturized deployable devices like clocks and sensors, these elements must ultimately be microfabricated, ideally monolithically with the trap to avoid losses associated with optical coupling between physically separate components. In this work we design, fabricate, and test an optical modulator capable of monolithic integration with a surface-electrode ion trap. These devices consist of piezo-optomechanical photonic integrated circuits configured as multi-stage Mach-Zehnder modulators that are used to control the intensity of light delivered to a single trapped ion on a separate chip. We use quantum tomography employing hundreds of multi-gate sequences to enhance the sensitivity of the fidelity to the types and magnitudes of gate errors relevant to quantum computing and better characterize the performance of the modulators, ultimately measuring single qubit gate fidelities that exceed 99.7%.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Demonstration of a MOT in a sub-millimeter membrane hole

Abstract We demonstrate the generation of a cold-atom ensemble within a sub-millimeter diameter hole in a transparent membrane, a so-called “membrane MOT”. With a sub-Doppler cooling process, the atoms trapped by the membrane MOT are cooled down to 10 $$\upmu$$ μ K. The atom number inside the unbridged/bridged membrane hole is about $$10^4$$ 10 4 to $$10^5$$ 10 5 , and the $$1/e^2$$ 1 / e 2 -diameter of the MOT cloud is about 180 $$\upmu$$ μ m for a 400 $$\upmu$$ μ m-diameter membrane hole. Such a membrane device can, in principle, efficiently load cold atoms into the evanescent-field optical trap generated by the suspended membrane waveguide for strong atom-light interaction and provide the capability of sufficient heat dissipation at the waveguide. This represents a key step toward the photonic atom trap integrated platform (ATIP).

74 ATOMIC AND MOLECULAR PHYSICS↗

Selective acoustic control of photon-mediated qubit-qubit interactions

Quantum technologies such as quantum sensing, quantum imaging, quantum communications, and quantum computing rely on the ability to actively manipulate the quantum state of light and matter. Quantum emitters, such as color centers trapped in solids, are a useful platform for the realization of elementary building blocks (qubits) of quantum information systems. In particular, the modular nature of such solid-state devices opens up the possibility to connect them into quantum networks and create nonclassical states of light shared among many qubits. The function of a quantum network relies on efficient and controllable interactions among individual qubits. In this context, we present a scheme where optically active qubits of differing excitation energies are mutually coupled via a dispersive interaction with a shared mode of an optical cavity. This generally off-resonant interaction is prohibitive of direct exchange of information among the qubits. However, we propose a scheme in which by acoustically modulating the qubit excitation energies it is, in fact, possible to tune to resonance a preselected pair of qubits and thus open a communication channel between them. This method potentially enables fast (approximately nanoseconds) and parallelizable on-demand control of a large number of physical qubits. In this work, we develop an analytical and a numerical theoretical model demonstrating this principle and suggest feasible experimental scenarios to test the theoretical predictions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

High-Fidelity Two-Qubit Gates Using a Microelectromechanical-System-Based Beam Steering System for Individual Qubit Addressing

In a large scale trapped atomic ion quantum computer, high-fidelity two-qubit gates need to be extended over all qubits with individual control. We realize and characterize high-fidelity two-qubit gates in a system with up to four ions using radial modes. The ions are individually addressed by two tightly focused beams steered using microelectromechanical system mirrors. We deduce a gate fidelity of 99.49(7)% in a two-ion chain and 99.30(6)% in a four-ion chain by applying a sequence of up to 21 two-qubit gates and measuring the final state fidelity. Our team characterizes the residual errors and discuss methods to further improve the gate fidelity towards values that are compatible with fault-tolerant quantum computation.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Molecular bond stabilization in the strong-field dissociation of O 2 +

We theoretically examine the rotational and vibrational dynamics of O 2 + molecular ions exposed to intense, short laser pulses for conditions realized in contemporary pump-probe experiments. We solve the time-dependent Schrödinger equation within the Born-Oppenheimer approximation for an initial distribution of randomly aligned molecular ions. For fixed peak intensities, our numerical results show that total, angle-integrated O 2 + → O( 3 P) + O + ( 4 S 0 ) dissociation yields do not monotonically increase with increasing infrared-probe pulse duration. We find this pulse-duration-dependent stabilization to be consistent with the transient trapping of nuclear probability density in a light-induced (bond-hardening) potential-energy surface and robust against rotational excitation. We analyze this stabilization effect and its underlying bond-hardening mechanism (i) in the time domain, by following the evolution of partial nuclear probability densities associated with the dipole-coupled O 2 + (a 4 Π u ) and O 2 + (f 4 Π g ) cationic states, and (ii) in the frequency domain, by examining rovibrational quantum-beat spectra for the evolution of the partial nuclear probability densities associated with these states. In this work, our analysis reveals the characteristic timescale for the bond-hardening mechanism in O 2 + and explains the onset of bond stabilization for sufficiently long pulse durations.

74 ATOMIC AND MOLECULAR PHYSICS↗

Silicon-On-Sapphire Metasurfaces Generate Arrays of Dark and Bright Traps for Neutral Atoms

We demonstrated crystalline silicon-on-sapphire (c-SOS) metasurfaces that convert a Gaussian beam into arrays of complex optical traps, including arrays of optical bottle beams that trap atoms in dark regions interleaved with bright tweezer arrays. The high refractive index and indirect band gap of crystalline silicon make it possible to design high-resolution near-infrared (λ > 700 nm) metasurfaces that can be manufactured at scale using CMOS-compatible processes. Compared with active components like spatial light modulators (SLMs) that have become widely used to generate trap arrays, metasurfaces provide an indefinitely scalable number of pixels, enabling large arrays of complex traps in a very small form factor, as well as reduced dynamic noise. To design metasurfaces that can generate three-dimensional bottle beams to serve as dark traps, we modified the Gerchberg-Saxton algorithm to enforce complex-amplitude profiles at the focal plane of the metasurface and to optimize the uniformity of the traps across the array. We fabricated and measured c-SOS metasurfaces that convert a Gaussian laser beam into arrays of bright traps, dark traps, and interleaved bright/dark traps.

Gerchberg-Saxton↗

Confinement and Collective Escape of Active Particles

Active matter broadly covers the dynamics of self-propelled particles. While the onset of collective behavior in homogenous active systems is relatively well understood, the effect of inhomogeneities such as obstacles and traps lacks overall clarity. Here, we study how interacting, self-propelled particles become trapped and released from a trap. We have found that captured particles aggregate into an orbiting condensate with a crystalline structure. As more particles are added, the trapped condensates escape as a whole. Our results shed light on the effects of confinement and quenched disorder in active matter.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Trapping of lithium atoms in a large hollow optical dipole trap

We describe the trapping of lithium atoms in an optical dipole trap about 1 mm in size, with a nearly rectangular potential. The trap has the shape of a cylinder with flat bases. The confinement region is bounded by thin walls produced by light with a frequency blue-detuned from an atomic transition (resonance) frequency by 19 GHz. Before trapping, the gas is collected and cooled in a magneto-optical trap whose centre nearly coincides with the centre of the dipole trap. After switching off the magneto-optical trap, we have photographed the atoms remaining in the dipole trap. (paper)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Sub-Doppler Cooling of a Trapped Ion in a Phase-Stable Polarization Gradient

Trapped ions provide a highly controlled platform for quantum sensors, clocks, simulators, and computers, all of which depend on cooling ions close to their motional ground state. Existing methods like Doppler, resolved sideband, and dark resonance cooling balance trade-offs between the final temperature and cooling rate. A traveling polarization gradient has been shown to cool multiple modes quickly and in parallel, but utilizing a stable polarization gradient can achieve lower ion energies, while also allowing tailorable light-matter interactions in the sub-wavelength regime. In this Letter, we demonstrate cooling of a trapped ion below the Doppler limit using a phase-stable polarization gradient created using trap-integrated photonic devices. At an axial frequency of 2⁢𝜋×1.45 MHz we achieve ⟨𝑛⟩=1.56±0.07 in 150 μ⁢s and cooling rates of ∼0.3 quanta/μ⁢s. Here, we examine ion dynamics under different polarization gradient phases, detunings, and intensities, showing reasonable agreement between experimental results and a multilevel model. Cooling is fast and power efficient, with lower average motional Fock state occupation when compared to simulated operation under the corresponding running wave configuration. Our results demonstrate a well-controlled test bed for studying the dynamics of multilevel atomic systems in a phase-stable polarization gradient.

Atom & ion cooling↗

Self‐Trapped and Free Exciton Dynamics in Vacuum‐Deposited Cesium Copper Iodide Thin Films

Abstract Highly photoluminescent, lead‐free perovskites are of interest for displays and solid‐state light‐emitting devices. In this report, streak camera‐based time‐resolved emission and transient absorption spanning visible to deep‐ultraviolet (UV) wavelengths are utilized to study self‐trapped and free exciton dynamics in vacuum‐deposited cesium copper halide thin films of CsCu 2 I 3 and Cs 3 Cu 2 I 5 . Self‐trapped exciton emission of CsCu 2 I 3 exhibits more noticeable changes with time in the peak position and width than Cs 3 Cu 2 I 5 . UV‐to‐blue emission is detectable for both compositions, where free exciton emission is distinct for CsCu 2 I 3 . Transient absorption shows loss of ground‐state bleach signals at early time delays for both, and the bleach signal shifts toward higher energy as time delay increases, likely due to strains induced by the newly created self‐trapped excitons. Global analysis performed on the transient absorption results yields time constants in these materials that build an overall dynamic scheme. This work aids in building a complete picture regarding light emission in these promising materials.

36 MATERIALS SCIENCE↗

Tunable broadband luminescence in lead-free hybrid copper halides

Metal halides are an important class of optoelectronic materials combining exceptional optical and electronic properties. An inherent advantage of metal halides is their solution synthesis and processability, which render them as low-cost and environmentally friendly materials for a range of applications from photovoltaics and photodetection to solid-state lighting (SSL). Here, in this study, we synthesized three previously unreported lead-free organic–inorganic hybrid copper halides: (OA) 4 CuX 5 (X = Br, I; OA + = C 8 H 17 NH 3+ , n-octylammonium cation) and (HA) 2 CuI 3 (HA + = C 6 H 13 NH 3 + , n-hexylammonium cation), all of which exhibit broadband emissions arising from self-trapped excitons (STEs). Among these compounds, (OA) 4 CuI 5 demonstrates tunable dual-band white-light emission with a high color rendering index value of 91 at room temperature. Temperature-dependent photoluminescence measurements and first-principles calculations reveal distinct behaviors between the two emission states in (OA) 4 CuI 5 . These findings highlight the potential of copper halide compounds for optoelectronic applications, particularly in the development of environmentally friendly solid-state lighting technologies.

36 MATERIALS SCIENCE↗

Hyperfine spectroscopy and laser cooling of the fermionic isotopes 47 Ti and 49 Ti

Here, we report on magneto-optical trapping of the two fermionic isotopes of atomic titanium, 47 Ti and 49 Ti . Unlike the even mass-number isotopes, which were recently laser cooled, 47 Ti and 49 Ti have nonzero nuclear spins and, consequently, their atomic levels are split by hyperfine structure. Combining and comparing theoretical calculations and atomic beam-spectroscopy measurements, we determine the hyperfine structures and isotope shifts of the 3⁢𝑑 2 ⁢4⁢𝑠 2 𝑎 3 ⁢𝐹 4 → 3⁢𝑑 2 ⁢( 3 𝑃)⁢4⁢𝑠⁢4⁢𝑝⁢( 3 𝑃 𝑜 ) 𝑦 5 ⁢𝐷$^o_4$ optical-pumping transition at optical wavelength 391 nm and the 3⁢𝑑 3 ⁢(4𝐹)⁢4⁢𝑠 𝑎 5 ⁢𝐹 5 → 3⁢𝑑 3 ⁢( 4 𝐹)⁢4⁢𝑝 𝑦 5 ⁢𝐺$^𝑜_6$ laser-cooling transition at wavelength 498 nm. With this information, we produce magneto-optical traps of both 47 Ti and 49 Ti by applying two additional tones of light to repump atoms to the maximum-spin states on the laser-cooling transition. Directly loading from the atomic flux of a titanium sublimation pump, we produce 47 Ti and 49 Ti traps with 731(190) and 1142(240) atoms, and with lifetimes of 330⁢(15) and 310⁢(8)⁢ ms, respectively.

atomic spectra↗

Light-induced Kondo-like exciton-spin interaction in neodymium(II) doped hybrid perovskite

Abstract Tuning the properties of a pair of entangled electron and hole in a light-induced exciton is a fundamentally intriguing inquiry for quantum science. Here, using semiconducting hybrid perovskite as an exploratory platform, we discover that Nd 2+ -doped CH 3 NH 3 PbI 3 (MAPbI 3 ) perovskite exhibits a Kondo-like exciton-spin interaction under cryogenic and photoexcitation conditions. The feedback to such interaction between excitons in perovskite and the localized spins in Nd 2+ is observed as notably prolonged carrier lifetimes measured by time-resolved photoluminescence, ~10 times to that of pristine MAPbI 3 without Nd 2+ dopant. From a mechanistic standpoint, such extended charge separation states are the consequence of the trap state enabled by the antiferromagnetic exchange interaction between the light-induced exciton and the localized 4 f spins of the Nd 2+ in the proximity. Importantly, this Kondo-like exciton-spin interaction can be modulated by either increasing Nd 2+ doping concentration that enhances the coupling between the exciton and Nd 2+ 4 f spins as evidenced by elongated carrier lifetime, or by using an external magnetic field that can nullify the spin-dependent exchange interaction therein due to the unified orientations of Nd 2+ spin angular momentum, thereby leading to exciton recombination at the dynamics comparable to pristine MAPbI 3 .

36 MATERIALS SCIENCE↗

Probing exciton diffusion dynamics in photosynthetic supercomplexes via exciton–exciton annihilation

Photosynthesis converts solar energy into chemical energy through coordinated energy transfer between light-harvesting complexes and reaction centers (RCs). Understanding exciton motion, particularly the exciton diffusion length, is essential for optimizing energy efficiency in photosystems. In this work, we combine intensity-cycling transient absorption spectroscopy with kinetic Monte Carlo (kMC) simulation to investigate exciton motion in the C2S2 photosystem II supercomplex of spinach. Using exciton–exciton annihilation, revealed in the fifth-order response, we experimentally estimate an exciton diffusion length of 10.9 nm based on a 3D normal diffusion model, suggesting the ability of excitons to traverse the supercomplex. However, kMC simulations reveal that exciton motion is sub-diffusive because of spatial constraints and the strong RC traps. An anomalous diffusion model analysis of the experimental data yields a diffusion length of 9.7 nm, while the simulated diffusion length is 7.4 nm. The variable exciton residence time across subunits, partly influenced by their connectivity to the trap, indicates inhomogeneous annihilation probability and suggests how plants balance efficient light harvesting with photoprotection. We also explore the influence of specific assumptions in the annihilation simulation, which are challenging to access in more complex environments, such as the thylakoid membrane. Our study provides a framework for studying exciton dynamics using exciton–exciton annihilation, which can be extended to understand the light-harvesting efficiencies of larger, more complex photosynthetic assemblies.

Zhang, Kunyan (ORCID:000000026830409X)↗