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Four-photon photoemission is observed from tungsten using carefully controlled and calibrated single pulses produced by a passively mode-locked Nd:YAG laser system. The results are shown to be in quantitative agreement with a four-photon generalization of the Fowler and DuBridge theories of photoemission.
An interface photodischarge study of p-type GaAs metal-oxide-semiconductor (MOS) structures revealed the presence of deep interface states and shallow donors and acceptors which were previously observed in n-type GaAs MOS through sub-band-gap photoionization transitions. For higher photon energies, internal photoemission was observed, i.e., injection of electrons to the conduction band of the oxide from either the metal (Au) or from the GaAs valence band; the threshold energies were found to be 3.25 and 3.7 + or - 0.1 eV, respectively. The measured photoemission current exhibited a thermal activation energy of about 0.06 eV, which is consistent with a hopping mechanism of electron transport in the oxide.
High quantum efficiency achieved without multiple layer contacts. Proposed infrared sensor based on photoemission from multiple layers of metal silicide sandwiched between layers of silicon. Suitable for use in focal-plane arrays. Layered internal-photoemission sensor has positive/intrinsic/negative structure modified by inclusion of layers or islands of metal silicide. Holes photo-excited from silicide regions and swept to detection by reverse-bias electric field in intrinsic silicon. Easier to make because internal layers allowed to "float" electrically, contact being made with only two outer semiconductor layers.
There is a major need for long-wavelength-infrared (LWIR) detector arrays in the range of 8 to 16 microns which operate with close-cycle cryocoolers above 65 K. In addition, it would be very attractive to have Si-based infrared (IR) detectors that can be easily integrated with Si readout circuitry and have good pixel-to-pixel uniformity, which is critical for focal plane array (FPA) applications. Here, researchers report a novel Si(1-x)Ge(x)/Si heterojunction internal photoemission (HIP) detector approach with a tailorable long wavelength infrared cutoff wavelength, based on internal photoemission over the Si(1-x)Ge(x)/Si heterojunction. The HIP detectors were grown by molecular beam epitaxy (MBE), which allows one to optimize the device structure with precise control of doping profiles, layer thickness and composition. The feasibility of a novel Si(1-x)Ge(x)/Si HIP detector has been demonstrated with tailorable cutoff wavelength in the LWIR region. Photoresponse at wavelengths 2 to 10 microns are obtained with quantum efficiency (QE) above approx. 1 percent in these non-optimized device structures. It should be possible to significantly improve the QE of the HIP detectors by optimizing the thickness, composition, and doping concentration of the Si(1-x)Ge(x) layers and by configuring the detector for maximum absorption such as the use of a cavity structure. With optimization of the QE and by matching the barrier energy to the desired wavelength cutoff to minimize the thermionic current, researchers predict near background limited performance in the LWIR region with operating temperatures above 65K. Finally, with mature Si processing, the relatively simple device structure offers potential for low-cost producible arrays with excellent uniformity.
A new SiGe/Si heterojunction internal photoemission (HIP) long-wavelength infrared (LWIR) detector has been fabricated by molecular beam epitaxy (MBE). The detection mechanism of the SiGe/Si HIP detector is infrared absorption in the degenerately doped p+-SiGe layer followed by internal photoemission of photoexcited holes over a heterojunction barrier. By adjusting the Ge concentration in the SiGe layer, and, consequently, the valence band offset between SiGe and Si, the cutoff wavelength of SiGe HIP detectors can be extended into the LWIR (8-17-micron) regime. Detectors were fabricated by growing p+-SiGe layers using MBE on patterned p-type Si substrates. The SiGe layers were boron-doped, with concentrations ranging from 10 to the 19th/cu cm to 4 x 10 to the 20th/cu cm. Infrared absorption of 5-25 percent in a 30-nm-thick p+-SiGe layer was measured in the 3-20-micron range using a Fourier transform infrared spectrometer. Quantum efficiencies of 3-5 percent have been obtained from test devices in the 8-12-micron range.
Cutoff wavelengths tailored by choice of Ge content. Infrared detectors based on internal photoemission at Si1-xGex/Si heterojunctions exhibited photoresponses at wavelengths from 2 to 12 micrometers in initial tests. Si1-xGex/Si-heterojunction internal-photoemission detectors tailored for use at wavelengths of order of 10 micrometers. Future developments expected to include integration of such devices with silicon readout circuitry to form infrared-imaging arrays. Imaging arrays operating in important wavelength range of 8 to 12 micrometers can be fabricated relatively inexpensively for use in outer-space, military, and industrial applications.
A laboratory experiment has been developed at Marshall Space Flight Center to study the interaction of micron-sized particles with plasmas and FUV radiation. The intent is to investigate the conditions under which particles of various compositions and sizes become charged, or discharged, while exposed to an electron beam and/or UV radiation. This experiment uses a unique laboratory where a single charged micron size particle is suspended in a quadrupole trap and then subjected to a controlled environment. Tests are performed using different materials and sizes, ranging from 10 microns to 1 micron, to determine the particle's charge while being subjected to an electron beam and /or UV radiation. The focus of this presentation will be on preliminary results from UV photoemission tests, but past results from electron beam, secondary electron emission tests will also be highlighted. A monochromator is used to spectrally resolve UV in the 120 nm to 300 nm range. This enables photoemission measurements as a function of wavelength. Electron beam tests are conducted using I to 3 micron sized aluminum oxide particles subjected to energies between 100 eV to 3 KeV. It was found that for both positive and negative particles the potential tended toward neutrality over time with possible equilibrium potentials between -0.8 Volts and 0.8 Volts.
Hybrid multiferroics such as BiFeO$_3$ (BFO) and La$_{0.7}$Sr$_{0.3}$MnO$_3$ (LSMO) heterostructures are highly interesting functional systems due to their complex electronic and magnetic properties. One of the key parameters influencing the emergent properties is the quality of interfaces, where varying interdiffusion lengths can give rise to different chemistry and distinctive electronic states. Here we report high-resolution depth resolved chemical and electronic investigation of BFO/LSMO superlattice using standing-wave hard X-ray photoemission spectroscopy in the first-order Bragg as well as near-total-reflection geometry. Our results show that the interfaces of BFO on top of LSMO are atomically abrupt, while the LSMO on top of BFO interfaces show an interdiffusion length of around 1.2 unit cells. The two interfaces also exhibit different chemical gradients, with the BFO/LSMO interface being Sr-terminated by a spectroscopically distinctive high binding energy component in Sr 2p core-level spectra, which is spatially contained within 1 unit cell from the interface. From the electronic point of view, unique valence band features were observed for bulk-BFO, bulk-LSMO and their interfaces. Our X-ray optical analysis revealed a unique electronic signature at the BFO/LSMO interface, which we attribute to the coupling between those respective layers. Valence band decomposition based on the Bragg-reflection standing-wave measurement also revealed the band alignment between BFO and LSMO layers. Our work demonstrates that standing-wave hard x-ray photoemission is a reliable non-destructive technique for probing depth-resolved electronic structure of buried layers and interfaces with sub-unit-cell resolution. Equivalent investigations can be successfully applied to a broad class of material such as perovskite complex oxides with emergent interfacial phenomena.
Time- and angle-resolved photoemission spectroscopy is a powerful probe of electronic band structures out of equilibrium. Tuning time and energy resolution to suit a particular scientific question has become an increasingly important experimental consideration. Many instruments use cascaded frequency doubling in nonlinear crystals to generate the required ultraviolet probe pulses. In this work, we demonstrate how calculations clarify the relationship between laser bandwidth and nonlinear crystal thickness contributing to experimental resolutions and place intrinsic limits on the achievable time-bandwidth product. Experimentally, we tune time and energy resolution by varying the thickness of nonlinear β-BaB 2 O 4 crystals for frequency upconversion, providing a flexible experiment design. We achieve time resolutions of 58–103 fs and corresponding energy resolutions of 55–27 meV. We propose a method to select crystal thickness based on desired experimental resolutions.
Few-layer thick MoSe 2 and WSe 2 possess non-trivial spin textures with sizable spin splitting due to the inversion symmetry breaking embedded in the crystal structure and strong spin–orbit coupling. Here, we report a spin-resolved photoemission study of MoSe 2 and WSe 2 thin film samples epitaxially grown on a bilayer graphene substrate. Furthermore, we only found spin polarization in the single- and trilayer samples—not in the bilayer sample—mostly along the out-of-plane direction of the sample surface. The measured spin polarization is found to be strongly dependent on the light polarization as well as the measurement geometry, which reveals intricate coupling between the spin and orbital degrees of freedom in this class of material.
The electronic structure of surfaces plays a key role in the properties of quantum devices. However, surfaces are also the most challenging to simulate and engineer. Here, in this work, the electronic structure of InAs(001), InAs(111), and InSb(110) surfaces is studied using a combination of density functional theory (DFT) and angle-resolved photoemission spectroscopy (ARPES). Large-scale first principles simulations are enabled by using DFT calculations with a machine-learned Hubbard U correction [npj Comput. Mater. 6, 180 (2020)]. To facilitate direct comparison with ARPES results, a “bulk unfolding” scheme is implemented by projecting the calculated band structure of a supercell surface slab model onto the bulk primitive cell. For all three surfaces, a good agreement is found between DFT calculations and ARPES. For InAs(001), the simulations clarify the effect of the surface reconstruction. Different reconstructions are found to produce distinctive surface states, which may be detected by ARPES with low photon energies. For InAs(111) and InSb(110), the simulations help elucidate the effect of oxidation. Owing to larger charge transfer from As to O than from Sb to O, oxidation of InAs(111) leads to significant band bending and produces an electron pocket, whereas oxidation of InSb(110) does not. The combined theoretical and experimental results may inform the design of quantum devices based on InAs and InSb semiconductors, for example, topological qubits utilizing the Majorana zero modes.
We have argued the anomalous spectra of angle-resolved photoemission of high-Tc cuprates, using quantized massive collective-gauge fields, from the field-theoretical point of view. The relation between the bosonic function of electric origin and the quantized massive collective-gauge fields has been discussed.
SrCuO 2 has long been considered a near-archetypal realization of a quasi-one-dimensional (1D) system of interacting electrons with short-range interactions. Within this framework, experimental observations - interpreted through the lens of the 1D Hubbard model - suggest that electron and hole excitations decay into two types of (unphysical) collective bosonic modes: "spinons", which carry the spin degree of freedom, and "holons", which carry the charge degree of freedom. This model, known as spin-charge separation, is most directly evidenced by angle-resolved photoemission spectroscopy (ARPES), where a photo-induced hole decays into a continuum of these excitations. Here we present an alternative perspective grounded in first-principles, self-consistent, and parameter-free many-body perturbation theory. In this revised quasiparticle framework, ARPES can be understood as a one-body effect arising from mild disorder in a long-range antiferromagnetic ground state. the emergence of the so-called spinon branch arises naturally from spin disorder, the anomalous linewidths are accurately captured, and we provide a compelling explanation for the spectral weight observed at the non-magnetic zone boundary. This reinterpretation provides a unified explanation for key experimental signatures previously attributed to spin-charge separation, including features observed in optical conductivity. Additionally, we show that SrCuO 2 exhibits a nontrivial interchain coupling that significantly influences both its one-particle and two-particle spectral functions. By comparing the spectral features of SrCuO 2 with those of La 2 CuO 4 , we argue that SrCuO 2 shares notable similarities with the two-dimensional cuprates-both being rooted in a common CuO 4 plaquette-based molecular orbital framework.
We present that angle-resolved photoemission spectroscopy (ARPES) is the key momentum-resolved technique for direct probing of the electronic structure of a material. However, since it is highly surface-sensitive, it has been applied to a relatively small set of complex oxides that can be easily cleaved in ultra-high vacuum. Here we describe a new multi-module system at Brookhaven National Laboratory (BNL) in which an oxide molecular beam epitaxy (OMBE) is interconnected with an ARPES and a spectroscopic-imaging scanning tunneling microscopy (SI-STM) module. This new capability largely expands the range of complex-oxide materials and artificial heterostructures accessible to these two most powerful and complementary techniques for studies of electronic structure of materials. Lastly, we also present the first experimental results obtained using this system — the ARPES studies of electronic band structure of a La 2-x Sr x CuO 4 (LSCO) thin film grown by OMBE.
Graphical abstract: The influence on the photoluminescent performance due to the electronic structure change in Eu-doped CaTiO{sub 3} of the specific core-level and valence band spectrum via X-ray photoemission spectroscopy were characterized. - Highlights: • Single phase CaTiO{sub 3} and CaTiO{sub 3}: Eu crystals were prepared under mild hydrothermal method. • Crystal structure, doping level and the relations to their luminescent property were discussed. • Charge compensation mechanism was discussed via valance band spectrum by XPS. - Abstract: Charge compensation of on-site Eu 4f–5d transition that determines the luminescent performance was confirmed with valance band spectrum. Influence of photoelectrons from CaTiO{sub 3}: Eu to the corresponding luminescent performance was discussed based on the crystal structure, doping level and the relations to their luminescent property. This paper is important to further optimize the luminescent performance for improving the efficiency and reducing the cost in light emitting diode industry.
Identifying thermodynamic signatures of electronic phases, such as superconductivity, is challenging in low-dimensional materials due to strong fluctuations and low probing volume. Spectroscopic methods are often used to identify new bulk phases, but their main measurable quantity—electronic energy gaps—is no longer an effective order parameter in low-dimensional and fluctuating systems. Combining angle-resolved photoemission with a domain-adversarial neural network, we report a data-driven method to identify thermodynamic phase transitions solely based on single-particle spectra. We demonstrate 97.6% accuracy in cuprate superconductor Bi 2 Sr 2 CaCu 2 O 8+δ with strong superconducting fluctuations. This model notably compensates for the scarcity of experimental data by leveraging virtually inexhaustible simulated data. Further, its explainability reveals the crucial role of in-gap spectral weight in detecting phase fluctuations and thermodynamic transitions. Our work pinpoints the spectroscopic signatures of fluctuating orders and enables using spectroscopy for machine-learning-assisted material discovery for low-dimensional and strong coupling systems.
Here, nano-patterned photocathodes (NPC) take advantage of plasmonic effects to resonantly increase absorption of light and localize electromagnetic field intensity on metal surfaces leading to surface-plasmon enhanced photoemission. In this paper, we report the status of NPC research at UCLA including in particular the optimization of the dimensions of a nanohole array on a silver wafer to enhance plasmonic response at 800 nm light, the development of a spectrally-resolved reflectivity measurement setup for quick nanopattern validation, and of a novel cathode plug to enable high power tests of NPCs on single crystal substrates in a high gradient radiofrequency gun.
Magnetically controlled states in quantum materials are central to their unique electronic and magnetic properties. However, direct momentum-resolved visualization of these states via angle-resolved photoemission spectroscopy (ARPES) has been hindered by the disruptive effect of magnetic fields on photoelectron trajectories. Here, we introduce an in situ method that is, in principle, capable of applying magnetic fields up to 1 T. This method uses substrates composed of nanomagnetic metamaterial arrays with alternating polarity. Such substrates can generate strong, homogeneous, and spatially confined fields applicable to samples with thicknesses up to the micron scale, enabling ARPES measurements under magnetic fields with minimal photoelectron trajectory distortion. Here, we demonstrate this minimal distortion with ARPES data taken on monolayer graphene. Our method paves the way for probing magnetic field-dependent electronic structures and studying field-tunable quantum phases with state-of-the-art energy-momentum resolutions.