Solid-state Quantum Research Articles

Ultrahighly-efficient and stable luminescent solar concentrators enabled by FRET-based carbon nanodots

Luminescent solar concentrators (LSCs) as an optical device to concentrate light from large areas illuminated by sunlight into small-area photovoltaic cells, can greatly reduce the cost of solar energy generation, thus showing promise in building-integrated photovoltaics. Here, we report the synthesis of a novel type of composite nanoparticle via the simple sol-gel method. Starting from hydroxyl-rich carbon nanodots (CDs), Rhodamine B (RhB) molecules were embedded into a silica matrix shell, forming a composite core-shell system, where the CDs represent the core and RhB embedded in SiO2 are the shell of the final CDs/RhB@SiO2 structure. These nanoparticles were successfully employed in high-performance LSC fabrication. The Förster resonant energy transfer (FRET) between the CDs and the dye was successfully exploited to improve the light absorption efficiency and power conversion efficiency (ηPCE) of LSC devices. The solid-state photoluminescence quantum yield of the as-synthesized composite nanoparticles can reach ∼ 57 % due to the effective suppression of the aggregation-induced quenching. These fluorescent composite nanoparticles were used for fabricating LSC devices with an ultrahigh ηPCE of ∼ 3.8 % for 5 × 5 cm2 devices, thanks to the high loading of luminophores and effective FRET.

High-dimensional spin-orbital single-photon sources.

Hybrid integration of solid-state quantum emitters (QEs) into nanophotonic structures opens enticing perspectives for exploiting multiple degrees of freedom of single-photon sources for on-chip quantum photonic applications. However, the state-of-the-art single-photon sources are mostly limited to two-level states or scalar vortex beams. Direct generation of high-dimensional structured single photons remains challenging, being still in its infancy. Here, we propose a general strategy to design highly entangled high-dimensional spin-orbital single-photon sources by taking full advantage of the spatial freedom to design QE-coupled composite (i.e., Moiré/multipart) metasurfaces. We demonstrate the generation of arbitrary vectorial spin-orbital photon emission in high-dimensional Hilbert spaces, mapping the generated states on hybrid-order Bloch spheres. We further realize single-photon sources of high-dimensional spin-orbital quantum emission and experimentally verify the entanglement of high-dimensional superposition states with high fidelity. We believe that the results obtained facilitate further progress in integrated solutions for the deployment of next-generation high-capacity quantum information technologies.

Controlling Energy Storage Crossing Quantum Phase Transitions in an Integrable Spin Quantum Battery.

We investigate the performance of a one-dimensional dimerized XY chain as a spin quantum battery. Such integrable model shows a rich quantum phase diagram that emerges through a mapping of the spins onto auxiliary fermionic degrees of freedom. We consider a charging protocol relying on the double quench of an internal parameter, namely the strength of the dimerization, and address the energy stored in the systems. We observe three distinct regimes, depending on the timescale characterizing the duration of the charging: a short-time regime related to the dynamics of the single dimers, a long-time regime related to the recurrence time of the system at finite size, and a thermodynamic limit time regime. In the latter, the energy stored is almost unaffected by the charging time and the precise values of the charging parameters, provided the quench crosses a quantum phase transition. Finally, we analytically prove that the three-timescale behavior and the strong dependence of the energy stored on the quantum phase diagram also hold in the quantum Ising chain in a transverse field. Our results can play a relevant role in the design of stable solid-state quantum batteries.

Quantum Carry Research of Q1D – SE on Helium at Charged Substrate

Known in nano-electronic a solid state quantum - size systems motivate they creating using the surface electrons over helium. The quantum carry of quasi-one-dimensional surface electrons (Q1D-SEs) over superfluid helium is considered here. Research performed according to an electron phase diagram in gas phase at conditions far from electron quantum melting. A substrate is dense row of the light-guide segments where the SEs channels are formed over helium in the fiber gaps. The electrostatic model of substrate profile demonstrates modulation of potential in the electric field leading to possibility of the fibers tops charge thereby improving the Q1D-SEs channels quality. The experiments carried out by a low - frequency electron transport method at the temperature from 1.5 K to 0.5 K and the concentrations of electrons were up to 109cm-2. The SE move transverse to channel satisfies conditions of quantization in sense both the temperature and the relaxation time of electron in a system. According to an experiment lower some temperature the SE conductivity is ladder-like. The differential of SE conductivity is peak-like corresponding qualitatively to an electron states density. The distance between peaks accords to the 1D energy spectrums in some approach. Possibility of apply the 1D-SEs quantized energy levels (vibration levels) as quantum bits of quantum computer is considered.

Qubit teleportation between a memory-compatible photonic time-bin qubit and a solid-state quantum network node

We report on a quantum interface linking a diamond NV center quantum network node and 795nm photonic time-bin qubits compatible with Thulium and Rubidium quantum memories. The interface makes use of two-stage low-noise quantum frequency conversion and waveform shaping to match temporal and spectral photon profiles. Two-photon quantum interference shows high indistinguishability between converted 795nm photons and the native NV center photons. We use the interface to demonstrate quantum teleportation including real-time feedforward from an unbiased set of 795nm photonic qubit input states to the NV center spin qubit, achieving a teleportation fidelity well above the classical bound. This proof-of-concept experiment shows the feasibility of interconnecting different quantum network hardware.

Numerical study of P3HT-based hybrid solid-state qantum dot solar cells with CdS quantum dots employing different metal oxides using SCAPS-1D

This study presents a comprehensive numerical investigation into solid-state quantum dot solar cells (SSQDSCs) utilizing P3HT poly(3-hexylthiophene) as both a hole transport and absorber layer employing SCAPS-1D simulation software, the research explores the performance of cells composed of FTO (Fluorine-doped Tin Oxide) as the front contact, integrated with different metal oxides (Titanium dioxide (TiO2), zinc oxide (ZnO), and tin dioxide (SnO2), CdS (Cadmium sulfide )quantum dots, P3HT, and Pt (platinum )as the back contact namely Hybrid solar cell. The thickness of each layer is systematically optimized, and the influence of various CdS quantum dots sizes is thoroughly examined. The study also dived into the characterization of interface defects at the P3HT/CdS junction, involving modifications to the electron affinity of P3HT. Additionally, the impact of metal work function variations was also investigated analyzing at each case critical parameters such as open-circuit voltage (VOC), short-circuit current density (JSC), fill factor (FF), power conversion efficiency (PCE) and quantum efficiency. The results demonstrate that optimization of these parameters has the potential to elevate solar cell efficiency to 18%. These simulation findings offer valuable insights for comparative analysis and a deeper understanding of the challenges encountered in experimental research.

Understanding the Role of NHC Ditopic Ligand Substituents in the Molecular Diversity and Emissive Properties of Silver Complexes.

Silver bis(carbene) complexes featuring ditopic N-heterocyclic carbene (NHC) ligands have been synthesized which enable the assembly of supramolecular architectures via reaction with silver triflate. Through a systematic exploration of crystal structures and emissive properties, this study investigates the impact of the substituents on the NHC ditopic ligands [R-Im-2-Z-py], where R = Me, benzyl (Bz), or 2-naphthylmethyl (NaphCH2), and Z = H or Cl in the structural framework and emissive properties observed in the silver bis(carbene) or polynuclear species. Remarkably diverse structural motifs emerge in both of them, predominantly influenced by the choice of R wingtip and second by the Z substituent. Also the emissive quantum yield of the complexes is mostly governed by the selection of the R wingtip and further modulated by the Z substituent. Several of the mono and polynuclear complexes exhibit complex emissive profiles, including the observation of dual emission phenomena. Particularly noteworthy is the complex [Ag(NHC)]2]OTf (R = Bz, Z = Cl), which demonstrates an exceptionally intense single blue emission with a remarkable solid-state quantum yield (Φ) of 24%.

Narrowband Electroluminescence from Color Centers in Hexagonal Boron Nitride.

Defects in wide bandgap materials have emerged as promising candidates for solid-state quantum optical technologies. Electrical excitation of single emitters may lead to scalable on-chip devices and therefore is highly sought after. However, most wide bandgap materials are not amenable to efficient doping, posing challenges for electrical excitation and on-chip integration. Here, we demonstrate narrowband electroluminescence from visible and near-infrared color centers in hexagonal boron nitride (hBN). We harness van der Waals tunnel junctions of graphene-hBN-graphene. Charge carriers are electrically injected into hBN, exciting localized defects that emit nonclassical light, as characterized by the second order correlation measurement. Remarkably, the devices operate at room temperature and produce robust, narrowband emission spanning from visible to the near-infrared. Our work marks an important milestone in vdW materials and their promising attributes for integrated quantum technologies and on-chip photonic circuits.

Mie metasurfaces for enhancing photon outcoupling from single embedded quantum emitters

Abstract Solid-state quantum emitters (QE) can produce single photons required for quantum information processing. However, their emission properties often exhibit poor directivity and polarisation definition resulting in considerable loss of generated photons. Here we propose and numerically evaluate Mie metasurface designs for outcoupling photons from an embedded and randomly-positioned QE. These Mie metasurface designs can provide over one order of magnitude enhancement in photon outcoupling with only several percent of photons being lost. Importantly, the Mie metasurfaces provide the enhancement in photon outcoupling without the need for strict QE position alignment and without affecting the intrinsic QE emission rate (Purcell enhancement). Electric dipole modes are key for achieving the enhancement and they offer a path for selective outcoupling for photons emitted with specific polarisation, including the out-of-plane polarisation. Mie metasurfaces can provide an efficient, polarisation-selective and scalable platform for QEs.

Strongly Enhanced Electronic Bandstructure Renormalization by Light in Nanoscale Strained Regions of Monolayer MoS2/Au(111) Heterostructures.

Understanding and controlling the photoexcited quasiparticle (QP) dynamics in monolayer (ML) transition metal dichalcogenides (TMDs) lays the foundation for exploring the strongly interacting, nonequilibrium two-dimensional (2D) QP and polaritonic states in these quantum materials and for harnessing the properties emerging from these states for optoelectronic applications. In this study, scanning tunneling microscopy/spectroscopy (STM/scanning tunneling spectroscopy) with light illumination at the tunneling junction is performed to investigate the QP dynamics in ML MoS2 on an Au(111) substrate with nanoscale corrugations. The corrugations on the surface of the substrate induce nanoscale local strain in the overlaying ML MoS2 single crystal, which result in energetically favorable spatial regions where photoexcited QPs, including excitons, trions, and electron-hole plasmas, accumulate. These strained regions exhibit pronounced electronic bandstructure renormalization as a function of the photoexcitation wavelength and intensity as well as the strain gradient, implying strong interplay among nanoscale structures, strain, and photoexcited QPs. In conjunction with the experimental work, we construct a theoretical framework that integrates nonuniform nanoscale strain into the electronic bandstructure of a ML MoS2 lattice using a tight-binding approach combined with first-principle calculations. This methodology enables better understanding of the experimental observation of photoexcited QP localization in the nanoscale strain-modulated electronic bandstructure landscape. Our findings illustrate the feasibility of utilizing nanoscale architectures and optical excitations to manipulate the local electronic bandstructure of ML TMDs and to enhance the many-body interactions of excitons, which is promising for the development of nanoscale energy-adjustable optoelectronic and photonic technologies, including quantum emitters and solid-state quantum simulators for interacting exciton polaritons based on engineered periodic nanoscale trapping potentials.

Single-Shot Readout and Weak Measurement of a Tin-Vacancy Qubit in Diamond

The negatively charged tin-vacancy center in diamond (SnV−) is an emerging platform for building the next generation of long-distance quantum networks. This is due to the SnV−’s favorable optical and spin properties including bright emission, insensitivity to electronic noise, and long spin coherence times at temperatures above 1 K. Here, we demonstrate measurement of a single SnV− electronic spin with a single-shot readout fidelity of 87.4%, which can be further improved to 98.5% by conditioning on multiple readouts. In the process, we develop understanding of the relationship between strain, magnetic field, spin readout, and microwave spin control. We show that high-fidelity readout is compatible with rapid microwave spin control, demonstrating a favorable parameter regime for use of the SnV− center as a high-quality spin-photon interface. Finally, we use weak quantum measurement to study measurement-induced dephasing; this illuminates the fundamental interplay between measurement and decoherence in quantum mechanics, and provides a universal method to characterize the efficiency of color-center spin readout. Taken together, these results overcome an important hurdle in the development of the SnV−-based quantum technologies and, in the process, develop techniques and understanding broadly applicable to the study of solid-state quantum emitters. Published by the American Physical Society 2024

Ultra-sensitive low-temperature luminescent thermometry based on Boltzmann behavior of the Stark sub-levels of Pr3+

The cryogenic sensor is critical for numerous applications such as cryobiology, aerospace space probes, and solid-state superconducting quantum technology. However, it is still a challenge to operate at temperatures below 100 K using luminescent intensity ratio (LIR) thermometers with typical thermal coupling levels based on the Boltzmann mechanism. In this work, a sensitive low-temperature luminescence thermometry approach has been developed utilizing Boltzmann behavior of the Stark sub-levels of Pr3+. Spectral Stark-splitting feature of the 1D2 multiplet of Pr3+ was observed in CaNb2O6: Pr3+ phosphor, and the luminescence intensity ratio (LIR) of high state (Stark sub-level (2)) and low state (Stark sub-level (0)) of 1D2 was employed for temperature sensing, resulting in a notable relative sensitivity (Sr) of 11.3 % K−1 at 60 K. In addition, the intervalence charge transfer (IVCT)-based strategy improves the temperature sensitivity above room temperature with maximum Sr up to 1.54 % K−1 at 420 K. This work consistently demonstrate high sensitivity at low temperature, indicating potential applications in cryogenic temperature sensor. These results provide a route to the development of luminescent thermometers with a high sensitivity at low temperatures and a wide range of operating temperatures.

Microwave Remote Sensing with Hybrid Quantum Receiver.

Detecting a microwave signal that is emitted or reflected by distant targets is a powerful tool in fundamental science and industrial technology. Solid-state spins provide an opportunity to realize quantum-enhanced remote sensing under ambient conditions. However, the weak interaction between the free-space signal and atomic size sensor limits the sensitivity. This hinders the realization of practical quantum remote sensing. Here, we demonstrate active microwave remote sensing with a diamond-based hybrid quantum receiver by combining electromagnetic field localization at nanoscale with quantum spin manipulation. A method of differential spin refocusing (DSR) is developed to overcome the challenge of reducing the impact of inhomogeneities in spin-signal interaction, while the strength of interaction is enhanced by more than 3 orders with nanostructure. It improves the coherent interaction time of quantum receiver by 30-fold, substantially enhancing the sensitivity and stability. By detecting the reflected microwave with picotesla sensitivity, diamond remote sensing monitors the real-time status of a centimeter-sized target at 2 m distance. Our method is general to various solid-state spins. The results will expand the applications of solid-state spin quantum sensors in areas ranging from medical imaging to resource survey.

Unraveling the Ultrasonic-Assisted Synthesis of Green-Emitting CsPbBr3@Cs4PbBr6: Reaction Process, Luminescence Property, and Display Application.

The pursuit of stable and highly emissive perovskite materials has garnered increasing attention in optoelectronic applications. Green-emitting CsPbBr3@Cs4PbBr6, as a green-emissive material in the solid-state form, has great potential as a color conversion material for full-color displays. However, it is a challenge to achieve mass preparation under ambient conditions. Meanwhile, the formation mechanism is ambiguous. This study reports a ligand-free and rapid mass synthesis of nanomicrosized CsPbBr3@Cs4PbBr6 solid via an ultrasonic-assisted method. The synthesized CsPbBr3@Cs4PbBr6 solids exhibit uniform morphology, high stability, and solid-state quantum efficiency of approximately 55%. Moreover, the transformation mechanism from Pb-Br complexes in the synthesis process is fully investigated by monitoring the phase and spectral evolution. By employing it as a green emitter, the obtained white light-emitting diode (LED) device shows high performance with a correlation color temperature of 7635 K and a wide color gamut of 123% NTSC. This study offers a low-cost and simple operation mass production method for solid-state perovskite powders with excellent chemical stability. Additionally, it provides new insights into the formation mechanism of highly efficient perovskite materials and promotes their practical applications.

Off-Normal Polarized Single-Photon Emission with Anisotropic Holography Metasurfaces.

Solid-state quantum emitters (QEs) with arbitrary direction emission and well-defined polarization are critical for scalable single-photon sources and quantum information processing. However, the design strategy for on-chip generation of off-normal photon emission with high-purity polarization characteristics has so far remained elusive. Here, we introduce the anisotropic holography metasurfaces for efficiently manipulating the emission direction and polarization of QE. The proposed method offers a flexible way to realize phase matching in surface plasmon scattering with spatially varying filling factors and provides an efficient route for designing advanced QE-coupled metasurfaces. By nonradiatively coupling nanodiamonds with metasurfaces, we experimentally demonstrate on-chip generation of well-collimated single-photon emission propagating along off-normal directions (i.e., 20° and 30°) featuring a divergence angle lower than 2.5°. The experimental average degree of linear polarization attains up to >0.98, thereby revealing markedly high polarization purity. This study facilitates applications of QEs in the deployment of integrated quantum networks.

Phonon engineering of atomic-scale defects in superconducting quantum circuits.

Noise within solid-state systems at low temperatures can typically be traced back to material defects. In amorphous materials, these defects are broadly described by the tunneling two-level systems (TLSs) model. TLS have recently taken on further relevance in quantum computing because they dominate the coherence limit of superconducting quantum circuits. Efforts to mitigate TLS impacts have thus far focused on circuit design, material selection, and surface treatments. Our work takes an approach that directly modifies TLS properties. This is achieved by creating an acoustic bandgap that suppresses all microwave-frequency phonons around the operating frequency of a transmon qubit. For embedded TLS strongly coupled to the transmon qubit, we measure a pronounced increase in relaxation time by two orders of magnitude, with the longest T1 time exceeding 5 milliseconds. Our work opens avenues for studying the physics of highly coherent TLS and methods for mitigating noise within solid-state quantum devices.

Aggregation Induced Emission-Based Covalent Organic Frameworks for High-Performance Optical Wireless Communication.

Here, we report the first utilization of covalent organic frameworks (COFs) in optical wireless communication (OWC) applications. In the solid form, aggregation-induced emission (AIE) luminogen often shows promising emissive characteristics that augment radiative decays and improve fluorescence. We have synthesized an AIE-COF through the Knoevenagel condensation reaction by taking advantage of the ability to carefully design and alter the COF structure by integrating an AIE luminogen with linear building blocks. The synthesized AIE-COF exhibited a high solid-state photoluminescence quantum yield (∼39%) and a short photoluminescence lifetime (∼1 ns), crucial for achieving modulation bandwidth for high-speed OWC applications. For comparison, we constructed an aggregation-caused quenching based COF, showing a similar lifetime but almost insignificant quantum yield. The orthogonal frequency-division multiplexing modulation strategy employed by the AIE-COF demonstrates remarkable high-rate data transmission, with a wide -3 dB modulation bandwidth of nearly 200 MHz and achieving high net data rates of 825 Mb/s, outperforming traditional materials. These results open new avenues for the ability to design and finetune new COF materials for their utilization as color converters in developing cutting-edge OWC components, enabling faster and more efficient data transfer.

π-Diamond: A Diamondoid Superstructure Driven by π-Interactions.

Modulating the arrangement of superstructures through noncovalent interactions has a significant impact on macroscopic shape and the expression of unique properties. Constructing π-interaction-driven hierarchical three-dimensional (3D) superstructures poses challenges on account of limited directional control and weak intermolecular interactions. Here we report the construction of a 3D diamondoid superstructure, named π-Diamond, employing a ditopic strained Z-shaped building block comprising a porphyrin unit as bow-limb double-strapped with two m-xylylene units as bowstrings. This superstructure, reminiscent of diamond's tetrahedral carbon composition, is composed of double-walled tetrahedron (DWT) driven solely by π-interactions. Hetero-π-stacking interactions between porphyrin and m-xylylene panels drive the assembly of four building blocks predominantly into a DWT, which undergoes extension to create an adamantane unit and eventually a diamondoid superstructure wherein each porphyrin panel is shared by two neighboring tetrahedra through hetero-π-stacking. π-Diamond exhibits a solid-state fluorescent quantum yield 44 times higher than that of tetraphenylporphyrin along with excellent photocatalytic performance. The precise 3D directionality of π-interactions, achieved through strained multipanel building blocks, revolutionizes the assembly of hierarchical 3D superstructures driven by π-interactions.

Synthesis and properties of chiral liquid crystal copolymers with tunable circularly polarized luminescence

Chiral liquid crystals have received widespread attention due to their unique advantages in improving circularly polarized luminescence (CPL) properties. However, how to achieve the emission and modulation of CPL for chiral liquid crystals within intrinsic polymer-based materials through a simple strategy remains a challenge. This article proposes a simple and feasible method to synthesize CPL chiral liquid crystals and manipulate their properties by copolymerizing chiral liquid crystal monomer with luminescent monomer. A series of intrinsic chiral luminescent liquid crystal copolymers C*(x)-Py(y) with tunable CPL performance were synthesized by copolymerizing chiral liquid crystal monomer MA6C* with pyrene-based luminescent monomer MC6Py in varying ratios. The effective control of the chiral liquid crystal phase structure and CPL performance of the copolymers C*(x)-Py(y) can be achieved by altering the composition of copolymers. In the copolymers, the CPL signal is generated due to the helix induction of pyrene chromophores by the chiral liquid crystals, and the CPL signal can be inverted and amplified by the unique selective reflection properties of chiral liquid crystals. For copolymer C*(0.75)-Py(0.25), the luminescence dissymmetry factor value and solid-state fluorescence quantum yield can reach −0.052 and 43.12%, respectively.

Tunable multi-peak emission solid-state fluorescent carbon dots: Luminescence regulation mechanism and application in single-component-based LEDs

The design of solid-state fluorescent carbon dots (CDs) with multi-peak emission has become an urgent challenge to be solved with the in-depth research of CDs in LEDs. Here, one- and two-component solid-state white light CDs are synthesized by microwave-assisted hydrothermal method using the biological pollutant cyanobacteria, respectively. The solid-state fluorescence quantum yield of the one-component CDs was as high as 41.8 %, and the solid-state fluorescence mechanism of CDs is discussed to be mainly attributed to the self-quenching-resistant feature of “core-shell” structure and the reabsorption/RET-induced long-wavelength red light emission, and attenuation of the short emission wavelength. For two-component white light CDs, blue- and red-light CDs are obtained by simple dialysis separation, realizing the fluorescence tunability. The different origins of their multi-peak emission are discussed: core, edge and surface states. The synthesis yields of CDs are up to 62 %, enabling stable gram-scale production. The white- and red-light CDs are used as phosphors to fabricate fluorescent films and cold, pure, and warm white- and red-light LEDs with good resistance to photobleaching and temperature stability and CRI of 84.4, 85.7 and 61.5.