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At least 757 records · Page 42

Free-Charge Carrier Generation in Homojunction Non-Polymeric Organic Semiconductor Films - The Role of the Optical Frequency Dielectric Constant

Engineering the dielectric constant (..epsilon..) to lower the exciton binding energy of the light-absorbing semiconductor can improve organic photovoltaic (OPV) device performance. Here, a series of materials are reported with 2-(3-oxo-2,3-dihydro-1H-inden-1-ylidene)malononitrile (INCN) acceptor end groups and a central glycolated bis(4H-cyclopenta[2,1-b:3,4-b']dithiophene) unit with large low-frequency (..epsilon..lf = 7.4-7.9 at 0.1-0.2 MHz) and optical-frequency (..epsilon..opt up to 6.6 at 2 x 1014 Hz) dielectric constants. The INCN end groups differed in whether they were protonated, chlorinated, or fluorinated, with the latter having the highest ..epsilon..opt. An ..epsilon..opt of 6.6 is predicted to lead to a low exciton binding energy of ~0.04 eV. Time-resolved microwave conductivity measurements showed a temperature-dependent yield-mobility product, with it increasing linearly from 340 K. The onset temperature was near that required to overcome the calculated exciton binding energy and indicates increased free charge generation in a homojunction film. Room temperature transient absorption spectroscopy revealed that photoexcitation rapidly converted to a lower energy state that was consistent with the formation of polarons or a charge transfer state. This work provides experimental evidence of the importance of ..epsilon..opt for the generation of free charges, and a strategy for development of efficient single chromophore homojunction OPV devices.

charge generation↗

Hardware-Efficient Quantum Phase Estimation via Local Control

Quantum phase estimation plays a central role in quantum simulation as it enables the study of spectral properties of many-body quantum systems. Most variants of the phase estimation algorithm require the application of the global unitary evolution conditioned on the state of one or more auxiliary qubits, posing a significant challenge for current quantum devices. In this work, we present an approach to quantum phase estimation that uses only locally controlled operations, resulting in a significantly reduced circuit depth. At the heart of our approach are efficient routines to measure the complex phase of the expectation value of the time-evolution operator, the so-called Loschmidt echo, for both circuit dynamics and Hamiltonian dynamics. By tracking changes in the phase during the dynamics, the routines trade circuit depth for increased sampling cost and classical postprocessing. Our approach does not rely on reference states and is applicable to any efficiently preparable state, regardless of its correlations. We provide a comprehensive analysis of the sample complexity and illustrate the results with numerical simulations. Our methods offer a practical pathway for measuring spectral properties in large many-body quantum systems using current quantum devices.

Schiffer, Benjamin F. [Max Planck Institute of Qua↗

Design of High-Performance Lead-Free Quaternary Antiperovskites for Photovoltaics via Ion Type Inversion and Anion Ordering

The emergence of halide double perovskites significantly increases the compositional space for lead-free and air-stable photovoltaic absorbers compared to halide perovskites. Nevertheless, most halide double perovskites exhibit oversized band gaps (>1.9 eV) or dipole-forbidden optical transition, which are unfavorable for efficient single-junction solar cell applications. The current device performance of halide double perovskite is still inferior to that of lead-based halide perovskites, such as CH 3 NH 3 PbI 3 (MAPbI 3 ). Here, by ion type inversion and anion ordering on perovskite lattice sites, two new classes of pnictogen-based quaternary antiperovskites with the formula of X 6 B 2 AA' and X 6 BB'A 2 are designed. Phase stability and tunable band gaps in these quaternary antiperovskites are demonstrated based on first-principles calculations. Further photovoltaic-functionality-directed screening of these materials leads to the discovery of 5 stable compounds (Ca 6 N 2 AsSb, Ca 6 N 2 PSb, Sr 6 N 2 AsSb, Sr 6 N 2 PSb, and Ca 6 NPSb 2 ) with suitable direct band gaps, small carrier effective masses and low exciton binding energies, and dipole-allowed strong optical absorption, which are favorable properties for a photovoltaic absorber material. The calculated theoretical maximum solar cell efficiencies based on these five compounds are all larger than 29%, comparable to or even higher than that of the MAPbI 3 based solar cell. Finally, our work reveals the huge potential of quaternary antiperovskites in the optoelectronic field and provides a new strategy to design lead-free and air-stable perovskite-based photovoltaic absorber materials.

three-dimensional electronic transport↗

Distributed measurement of minimum and maximum in-situ stress in substrates

A system for performing distributed measurements of in-situ stress includes an expandable element with at least one fiber optic sensor. The expandable element can be positioned at various depths in a hole in a substrate. A pressurizing device expands (and contracts) the expandable element when the expandable element is inserted in the hole in the substrate to exert pressure on the hole wall. A pressure sensor provides a sensor output indicative of a pressure applied to the hole wall by the expandable element. The fiber optic sensor and an optical interrogator measure strain along a length of the sensor in a continuous, high spatial resolution manner Based on the measured strain and pressure sensor output, the system determines various properties of the substrate such as, minimum principal stress, maximum principal stress, and/or principal stress direction associated with one or more fractures in the substrate, as well as substrate modulus.

Ohanian, III, Osgar John↗

All-Carbon Nanotube Solar Cell Devices Mimic Photosynthesis

We report that both solar cells and photosynthetic systems employ a two-step process of light absorption and energy conversion. In photosynthesis, they are performed by distinct proteins. However, conventional solar cells use the same semiconductor for optical absorption and electron-hole separation, leading to inefficiencies. Here, we show that an all-semiconducting single-walled carbon nanotube (s-SWCNTs) device provides an artificial system that models photosynthesis in a tandem geometry. We use distinct chirality s-SWCNTs to separate the site and direction of light absorption from those of power generation. Using different bandgap s-SWCNTs, we implement an energy funnel in dual-gated p-n diodes. The device captures photons from multiple regions of the solar spectrum and funnels photogenerated excitons to the smallest bandgap s-SWCNT layer, where they become free carriers. We demonstrate an increase in the photoresponse by adding more s-SWCNT layers of different bandgaps without a corresponding deleterious increase in the dark leakage current.

14 SOLAR ENERGY↗

Progress toward picosecond on-chip magnetic memory

Here, we offer a perspective on the prospects of ultrafast spintronics and opto-magnetism as a pathway to high-performance, energy-efficient, and non-volatile embedded memory in digital integrated circuit applications. Conventional spintronic devices, such as spin-transfer-torque magnetic-resistive random-access memory (STT-MRAM) and spin–orbit torque MRAM, are promising due to their non-volatility, energy-efficiency, and high endurance. STT-MRAMs are now entering into the commercial market; however, they are limited in write speed to the nanosecond timescale. Improvement in the write speed of spintronic devices can significantly increase their usefulness as viable alternatives to the existing CMOS-based devices. In this article, we discuss recent studies that advance the field of ultrafast spintronics and opto-magnetism. An optimized ferromagnet–ferrimagnet exchange-coupled magnetic stack, which can serve as the free layer of a magnetic tunnel junction (MTJ), can be optically switched in as fast as ~3 ps. Integration of ultrafast magnetic switching of a similar stack into an MTJ device has enabled electrical readout of the switched state using a relatively larger tunneling magnetoresistance ratio. Purely electronic ultrafast spin–orbit torque induced switching of a ferromagnet has been demonstrated using ~6 ps long charge current pulses. We conclude our Perspective by discussing some of the challenges that remain to be addressed to accelerate ultrafast spintronics technologies toward practical implementation in high-performance digital information processing systems.

42 ENGINEERING↗

Bistable Optical Semiconductor Switching Based on C-Doped GaN

Highly resistive gallium nitride (GaN) is an essential material for power optoelectronic applications. While carbon doping is widely used to achieve semi-insulating properties in GaN, the persistent photoconductivity (PPC) arising from deep-level defect traps remains a major obstacle for high-speed power switching. This study demonstrates a novel approach: leveraging the ultrahigh photoresponsivity of GaN:C (up to 2.1 A ⋅ cm/W ⋅ kV, surpassing alternatives such as GaN:Fe) and employing defect-selective optical control to effectively quench the PPC. By synchronizing a short infrared (1064 nm) quenching pulse with UV (385 nm) excitation in an epitaxially grown GaN:C layer on a heavily doped n-type GaN substrate, we achieve a dramatic reduction in photocurrent fall time by approximately 293× (from 470 to 1.6 μ s), increasing modulation bandwidth from 745 Hz to nearly 218 kHz. Here, this advancement not only establishes a new pathway for controlling PPC in GaN:C but also enables the practical integration of GaN:C in fast power switching devices. Enhanced modulation bandwidth, along with GaN:C excellent photoresponsivity, makes it a promising candidate for optically controlled high-voltage, high-power electronic systems, such as photoconductive semiconductor switches (PCSSs) used in pulsed-power drivers, high-power microwave (HPM) sources, and high-voltage gate drivers for wide bandgap (WBG) power electronics.

Carbon-dopped Gallium nitride (GaN:C)↗

Implementing the donor–acceptor approach in electronically conducting copolymers via electropolymerization

Electropolymerization has become a convenient method for synthesizing and characterizing complex organic copolymers having intrinsic electronic conductivity, including the donor (D)–acceptor (A) class of electronically conducting polymers (ECPs). This review begins with an introduction to the electrosynthesis of common second-generation ECPs. The information obtainable from electroanalytical studies, charge carriers such as polarons (positive and negative) and bipolarons (positive and negative) and doping will be discussed. The evolutionary chain of ECPs is then presented. ECPs comprising electron-rich D and electron-deficient A moieties have been shown to possess intrinsic electronic conductivity and unique optical and electronic properties. They are third generation ECPs and electropolymerization of mixtures of D and A leads to stoichiometrically controlled block copolymers. These D–A type ECPs are discussed on the basis of selected representative materials. Since the discovery of electropolymerization as a powerful tool to synthesize copolymers of conjugated monomers with a pre-determined ratio of D and A repeat units present in the polymer, the field of D–A type ECPs has grown considerably and the literature available since 2004 to 2021 is summarized and tabulated. Electronic and optical properties of the materials determined by computational chemistry are presented. The data obtained from electrochemical and optical methods are compared with those obtained from computational methods and reasons for discrepancies are given. The literature on the concept of electropolymerization extended to synthesizing triblock and many-block copolymers is reviewed. Finally, applications of D–A polymers in optoelectronic devices (organic solar cells and field-effect transistors) and in bio-imaging are explained quoting appropriate examples.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Optical and magneto-optical properties of ferromagnetic monolayer CrBr 3 : A first-principles G W and G W plus Bethe-Salpeter equation study

The discovery of atomically thin two-dimensional (2D) magnetic semiconductors has triggered enormous research interest recently. In this paper, we use first-principles many-body perturbation theory to study a prototypical 2D ferromagnetic semiconductor, monolayer chromium tribromide (CrBr 3 ). With broken time-reversal symmetry, spin-orbit coupling, and excitonic effects included through the full-spinor GW and GW plus Bethe-Salpeter equation (GW-BSE) methods, we compute the frequency-dependent layer polarizability tensor and dielectric function tensor that govern the optical and magneto-optical (MO) properties. In addition, we provide a detailed theoretical formalism for simulating magnetic circular dichroism, MO Kerr effect, and Faraday effect, demonstrating the approach with monolayer CrBr 3 . Due to reduced dielectric screening in 2D and the localized nature of the Cr d orbitals, we find strong self-energy effects on the quasiparticle band structure of monolayer CrBr 3 that give a 3.8 eV indirect bandgap. Also, excitonic effects dominate the low-energy optical and MO responses in monolayer CrBr 3 where a large exciton binding energy of 2.3 eV is found for the lowest bright exciton state with excitation energy at 1.5 eV. We further find that the MO signals demonstrate strong dependence on the excitation frequency and substrate refractive index. Furthermore, our theoretical framework for modeling optical and MO effects could serve as a powerful theoretical tool for future study of optoelectronic and spintronics devices consisting of van der Waals 2D magnets.

36 MATERIALS SCIENCE↗

Embrace the darkness: An experimental perspective on organic exciton–polaritons

Organic polaritonics has emerged as a captivating interdisciplinary field that marries the complexities of organic photophysics with the fundamental principles of quantum optics. By harnessing strong light–matter coupling in organic materials, exciton–polaritons offer unique opportunities for advanced device performance, including enhanced energy transport and low-threshold lasing, as well as new functionalities like polariton chemistry. In this review, we delve into the foundational principles of exciton–polaritons from an experimental perspective, highlighting the key states, processes, and timescales that govern polariton phenomena. Our review centers on the spectroscopy of exciton–polaritons. We overview the primary spectroscopic approaches that reveal polariton phenomena, and we discuss the challenges in disentangling polaritonic signatures from spectral artifacts. We discuss how organic materials, due to their complex photophysics and disordered nature, not only present challenges to the conventional polariton models but also provide opportunities for new physics, like manipulating dark electronic states. As the research field continues to grow, with increasingly complex materials and devices, this review serves as a valuable introductory guide for researchers navigating the intricate landscape of organic polaritonics.

36 MATERIALS SCIENCE↗

Efficient Optical Control of Magnon Dynamics in van der Waals Ferromagnets

Optical control of magnons in two-dimensional (2D) materials promises new functionalities for spintronics and magnonics in atomically thin devices. Here, we report control of magnon dynamics, using laser polarization, in a ferromagnetic van der Waals (vdW) material, Fe 3.6 Co 1.4 GeTe 2 . The magnon amplitude, frequency, and lifetime are controlled and monitored by time-resolved pump-probe spectroscopy. We show substantial (over 25%) and continuous modulation of magnon dynamics as a function of incident laser polarization. Our results suggest that the modification of the effective demagnetization field and magnetic anisotropy by the pump laser pulses with different polarizations is due to anisotropic optical absorption. This implies that pump laser pulses modify the local spin environment, which enables the launch of magnons with tunable dynamics. Our first-principles calculations confirm the anisotropic optical absorption of different crystal orientations. Our findings suggest a new route for the development of opto-spintronic or opto-magnonic devices.

36 MATERIALS SCIENCE↗

Second-harmonic generation tensors from high-throughput density-functional perturbation theory

Optical materials play a key role in enabling modern optoelectronic technologies in a wide variety of domains such as the medical or the energy sector. Among them, nonlinear optical crystals are of primary importance to achieve a broader range of electromagnetic waves in the devices. However, numerous and contradicting requirements significantly limit the discovery of new potential candidates, which, in turn, hinders the technological development. In the present work, the static nonlinear susceptibility and dielectric tensor are computed via density-functional perturbation theory for a set of 579 inorganic semiconductors. The computational methodology is discussed and the provided database is described with respect to both its data distribution and its format. Several comparisons with both experimental and ab initio results from literature allow to confirm the reliability of our data. The aim of this work is to provide a relevant dataset to foster the identification of promising nonlinear optical crystals in order to motivate their subsequent experimental investigation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Optically induced quantum transitions in direct probed mesoscopic NbSe 2 for prototypical bolometers

Superconducting transition-edge sensors (TES) have emerged as fascinating devices to detect broadband electromagnetic radiation with low thermal noise. The advent of metallic transition metal dichalcogenides, such as NbSe 2 , has also created an impetus to understand their low-temperature properties, including superconductivity. Interestingly, NbSe 2 -based sensor within the TES framework remains unexplored. In this work, direct-probed superconducting NbSe 2 absorbers led to a proof-of-concept demonstration for the transduction of incoming light to heat, where a thermodynamic superconducting phase transition in NbSe 2 was evident to switch it to the normal-state, when biased below its superconducting transition temperature. A wavelength-dependent response of its optical absorption properties was observed, based on the incident optical excitation source used. Furthermore, extensive optical characterization studies were conducted using Raman spectroscopy, where the in-plane and out-of-plane thermal conductivity was empirically determined. Our results open new possibilities for the use of NbSe 2 in superconducting radiation detectors, including in a TES framework

47 OTHER INSTRUMENTATION↗

Low-loss adiabatic fiber-optic coupler for cryogenic photonics

Recent developments in quantum light–matter coupled systems and quantum transducers have highlighted the need for cryogenic optical measurements. In this study, we present a packaged fiber-optic coupler with a coupling efficiency of over 50% for telecom wavelength light down to the mK temperature range. Besides the high coupling efficiency, our method enables sensitive photonic device measurements that are immune to mechanical vibrations present in cryogenic setups.

Optics↗

Ultrafast Control of Interfacial Exchange Coupling in Ferromagnetic Bilayer

Fast spin manipulation in magnetic heterostructures, where magnetic interactions between different materials often define the functionality of devices, is a key issue in the development of ultrafast spintronics. Although recently developed optical approaches such as ultrafast spin-transfer and spin–orbit torques open new pathways to fast spin manipulation, these processes do not fully utilize the unique possibilities offered by interfacial magnetic coupling effects in ferromagnetic multilayer systems. Here, ultrafast optically controlled interfacial exchange interactions in the ferromagnetic Co 2 FeAl/(Ga,Mn)As system at low laser fluence levels are experimentally demonstrated. The excitation efficiency of Co 2 FeAl with the (Ga,Mn)As layer is 30–40 times higher than the case with the GaAs layer at 5 K due to the modification of exchange coupling interaction via photoexcited charge transfer between the two ferromagnetic layers. In addition, the coherent spin precessions persist to room temperature, excluding the drive of pump-modulated magnetization in the (Ga,Mn)As layer and indicating a proximity-effect-related optical excitation mechanism. The results highlight the importance of interfacial exchange interactions in ferromagnetic heterostructures and how these magnetic coupling effects can be utilized for ultrafast, low-power spin manipulation.

36 MATERIALS SCIENCE↗

Low‐Temperature Synthesis of Stable CaZn 2 P 2 Zintl Phosphide Thin Films as Candidate Top Absorbers

Abstract The development of tandem photovoltaics and photoelectrochemical solar cells requires new absorber materials with bandgaps in the range of ≈1.5–2.3 eV, for use in the top cell paired with a narrower‐gap bottom cell. An outstanding challenge is finding materials with suitable optoelectronic and defect properties, good operational stability, and synthesis conditions that preserve underlying device layers. This study demonstrates the Zintl phosphide compound CaZn 2 P 2 as a compelling candidate semiconductor for these applications. Phase‐pure, ≈500 nm‐thick CaZn 2 P 2 thin films are prepared using a scalable reactive sputter deposition process at growth temperatures as low as 100 °C, which is desirable for device integration. Ultraviolet‐visible spectroscopy shows that CaZn 2 P 2 films exhibit an optical absorptivity of ≈10 4 cm −1 at ≈1.95 eV direct bandgap. Room‐temperature photoluminescence (PL) measurements show near‐band‐edge optical emission, and time‐resolved microwave conductivity (TRMC) measurements indicate a photoexcited carrier lifetime of ≈30 ns. CaZn 2 P 2 is highly stable in both ambient conditions and moisture, as evidenced by PL and TRMC measurements. Experimental data are supported by first‐principles calculations, which indicate the absence of low‐formation‐energy, deep intrinsic defects. Overall, this study shall motivate future work integrating this potential top cell absorber material into tandem solar cells.

14 SOLAR ENERGY↗

Room-Temperature Ferroelectric Epitaxial Nanowire Arrays with Photoluminescence

The development of large-scale, high-quality ferroelectric semiconductor nanowire arrays with interesting light-emitting properties can address limitations in traditional wide-bandgap ferroelectrics, thus serving as building blocks for innovative device architectures and next-generation high-density optoelectronics. Here, we investigate the optical properties of ferroelectric CsGeX 3 (X = Br, I) halide perovskite nanowires that are epitaxially grown on muscovite mica substrates by vapor phase deposition. Detailed structural characterizations reveal an incommensurate heteroepitaxial relationship with the mica substrate. Furthermore, photoluminescence that can be tuned from yellow-green to red emissions by varying the halide composition demonstrates that these nanowire networks can serve as platforms for future optoelectronic applications. In addition, the room-temperature ferroelectricity and ferroelectric domain structures of these nanowires are characterized using second harmonic generation (SHG) polarimetry. Finally, the combination of room-temperature ferroelectricity with photoluminescence in these nanowire arrays unlocks new avenues for the design of novel multifunctional materials.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Thickness-Dependent Cross-Plane Thermal Conductivity Measurements of Exfoliated Hexagonal Boron Nitride

Submicrometer-thick layers of hexagonal boron nitride (hBN) exhibit high in-plane thermal conductivity and useful optical properties, and serve as dielectric encapsulation layers with low electrostatic inhomogeneity for graphene devices. Despite the promising applications of hBN as a heat spreader, the thickness dependence of its cross-plane thermal conductivity is not known, and the cross-plane phonon mean free paths (MFPs) have not been measured. We measure the cross-plane thermal conductivity of hBN flakes exfoliated from bulk crystals. We find that submicrometer thick flakes exhibit thermal conductivities up to 8.1 ± 0.5 W m –1 K –1 at 295 K, which exceeds previously reported bulk values by more than 60%. Surprisingly, the average phonon mean free path is found to be several hundred nanometers at room temperature, a factor of 5 larger than previous predictions. When planar twist interfaces are introduced into the crystal by mechanically stacking multiple thin flakes, the cross-plane thermal conductivity of the stack is found to be a factor of 7 below that of individual flakes with similar total thickness, thus providing strong evidence that phonon scattering at twist boundaries limits the maximum phonon MFPs. These results have important implications for hBN integration in nanoelectronics and improve our understanding of thermal transport in twodimensional materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗