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At least 325 records · Page 18

Giant topological longitudinal circular photo-galvanic effect in the chiral multifold semimetal CoSi

The absence of mirror symmetry, or chirality, is behind striking natural phenomena found in systems as diverse as DNA and crystalline solids. A remarkable example occurs when chiral semimetals with topologically protected band degeneracies are illuminated with circularly polarized light. Under the right conditions, the part of the generated photocurrent that switches sign upon reversal of the light’s polarization, known as the circular photo-galvanic effect, is predicted to depend only on fundamental constants. The conditions to observe quantization are non-universal, and depend on material parameters and the incident frequency. In this work, we perform terahertz emission spectroscopy with tunable photon energy from 0.2 –1.1 eV in the chiral topological semimetal CoSi. We identify a large longitudinal photocurrent peaked at 0.4 eV reaching ~550 μ A/V 2 , which is much larger than the photocurrent in any chiral crystal reported in the literature. Using first-principles calculations we establish that the peak originates only from topological band crossings, reaching 3.3 ± 0.3 in units of the quantization constant. Our calculations indicate that the quantized circular photo-galvanic effect is within reach in CoSi upon doping and increase of the hot-carrier lifetime. The large photo-conductivity suggests that topological semimetals could potentially be used as novel mid-infrared detectors.

79 ASTRONOMY AND ASTROPHYSICS↗

Chirality manipulation of ultrafast phase switches in a correlated CDW-Weyl semimetal

Light engineering of correlated states in topological materials provides a new avenue of achieving exotic topological phases inaccessible by conventional tuning methods. Here we demonstrate a light control of correlation gaps in a model charge-density-wave (CDW) and polaron insulator (TaSe 4 ) 2 I recently predicted to be an axion insulator. Our ultrafast terahertz photocurrent spectroscopy reveals a two-step, non-thermal melting of polarons and electronic CDW gap via the fluence dependence of a longitudinal circular photogalvanic current. This helicity-dependent photocurrent reveals continuous ultrafast phase switches from the polaronic state to the CDW (axion) phase, and finally to a hidden Weyl phase as the pump fluence increases. Additional distinctive attributes aligning with the light-induced switches include: the mode-selective coupling of coherent phonons to the polaron and CDW modulation, and the emergence of a non-thermal chiral photocurrent above the pump threshold of CDW-related phonons. The demonstrated ultrafast chirality control of correlated topological states here holds large potentials for realizing axion electrodynamics and advancing quantum-computing applications.

36 MATERIALS SCIENCE↗

Vanishing carrier-envelope-phase-sensitive response in optical-field photoemission from plasmonic nanoantennas

At the surfaces of nanostructures, enhanced electric fields can drive optical-field photoemission and thereby generate and control electrical currents at frequencies exceeding 100 THz. A hallmark of such optical-field photoemission is the sensitivity of the total emitted current to the carrier-envelope phase (CEP). In this work, we examine CEP-sensitive photoemission from plasmonic gold nanoantennas excited with few-cycle optical pulses. At a critical pulse energy, which we call a vanishing point, we observe a pronounced dip in the magnitude of the CEP-sensitive photocurrent accompanied by a sudden shift of π radians in the photocurrent phase. Analysis shows that this vanishing behaviour arises due to competition between sub-optical-cycle electron emission events from neighbouring optical half-cycles and that both the dip and phase shift are highly sensitive to the precise shape of the driving optical waveform at the surface of the emitter. As the mechanisms underlying the dip and phase shift are a general consequence of nonlinear, field-driven photoemission, they may be used to probe sub-optical-cycle emission processes from solid-state emitters, atoms and molecules. Improved understanding of these CEP-sensitive photocurrent features will be critical to the development of optical-field-driven photocathodes for time-domain metrology and microscopy applications demanding attosecond temporal and nanometre spatial resolution.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

MoS 2 Heterojunctions by Thickness Modulation

In this work, we report lateral heterojunction formation in as-exfoliated MoS 2 flakes by thickness modulation. Kelvin probe force microscopy is used to map the surface potential at the monolayer-multilayer heterojunction, and consequently the conduction band offset is extracted. Scanning photocurrent microscopy is performed to investigate the spatial photocurrent response along the length of the device including the source and the drain contacts as well as the monolayer-multilayer junction. The peak photocurrent is measured at the monolayer-multilayer interface, which is attributed to the formation of a type-I heterojunction. Finally, the work presents experimental and theoretical understanding of the band alignment and photoresponse of thickness modulated MoS 2 junctions with important implications for exploring novel optoelectronic devices.

36 MATERIALS SCIENCE↗

Textured Nanoporous Mo:BiVO4 Photoanodes with High Charge Transport and Charge Transfer Quantum Efficiencies for Oxygen Evolution

We have developed a simple spin coating method to make high-quality nanoporous photoelectrodes of monoclinic BiVO4 and studied the ability of these electrodes to transport photogenerated carriers to oxidize sulfite and water. Samples containing molybdenum and featuring [001] out-of-plane crystallographic texture show a photocurrent and external quantum efficiency (EQE) for sulfite oxidation as high as 3.1 mA cm-2 and 60%, respectively, at 1.23 V versus reversible hydrogen electrode. By using an optical model of the electrode stack to accurately determine the fraction of electrode absorptance due to the BiVO4 active layer, we estimate that on average 70 +/- 5% of all photogenerated carriers escape recombination. A comparison of internal quantum efficiency as a function of film processing, illumination direction, and film thickness shows that electron transport is efficient and hole transport limits the photocurrent (hole diffusion length <40 nm). We find that Mo addition primarily improves electron transport and texturing mostly improves hole transport. Mo enhances electron transport by thinning the surface depletion layer or passivating traps and recombination centers at grain boundaries and interfaces, while improved hole transport in textured films may result from more efficient lateral hole extraction due to the texturing itself or the reduced density of deep gap states observed in photoemission measurements. Photoemission data also reveal that the films have bismuth-rich, vanadium- and oxygen-deficient surface layers, while ion scattering spectroscopy indicates a Bi-V-O surface termination. Without added catalysts, the plain BiVO4 electrodes oxidized water with an initial photocurrent and peak EQE of 1.7 mA cm-2 and 30%, respectively, which equates to a hole transfer efficiency to water of >64% at 1.23 V. The electrodes quickly photocorrode during water oxidation but show good stability during sulfite oxidation and indefinite stability in the dark. By improving the hole transport efficiency and coating these nanoporous BiVO4 films with an appropriate protective layer and oxygen evolution catalyst, it should be possible to achieve highly efficient and stable water oxidation at a practical pH.

36 MATERIALS SCIENCE↗

Creating stable interfaces between reactive materials: titanium nitride protects photoabsorber–catalyst interface in water-splitting photocathodes

The development of a solar-driven water splitting device that replaces costly precious metals, while achieving stable high performance, is a major challenge. Transition metal phosphides are active and low-cost catalysts for the hydrogen evolution reaction (HER), although, none thus far have exhibited stable performance when interfaced with semiconductors. In this work, we report on a monolithic junction consisting of cubic-NiP 2 :TiN:Si, fabricated using both commercial and custom Si photovoltaics. Stable performance is achieved using an ultrathin film of crystalline TiN that effectively hinders atomic diffusion between interfaces during fabrication. Crystalline cubic-NiP 2 deposited on TiN/n + p-Si retains 97% of the bare Si photovoltage, comparable saturation current density to bare Si, and has a turnover frequency of 1.04 H 2 per site per s at -100 mV applied potential. In acid, it requires only -150 mV additional overpotential compared to the benchmark, Pt/TiN/n + p-Si, to reach a HER photocurrent density of -10 mA cm -2 . This photocathode maintains a stable H 2 photocurrent (±10%) for at least 125 hours, the duration of testing. When the same layers are fabricated on a commercial Si solar cell, this photocathode produced double the photocurrent density (36.3 mA cm -2 , under simulated 1.5 AM G illumination). Physical characterization gives detailed information on the properties responsible for the observed activity and durability of these interfaces. In general, the thin-film methodology presented here is widely applicable, demonstrates superior activity, and achieves long-term stability.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

High broadband photoconductivity of few-layered MoS 2 field-effect transistors measured using multi-terminal methods: effects of contact resistance

Among the layered two dimensional semiconductors, molybdenum disulfide (MoS 2 ) is considered to be an excellent candidate for applications in optoelectronics and integrated circuits due to its layer-dependent tunable bandgap in the visible region, high ON/OFF current ratio in field-effect transistors (FET) and strong light–matter interaction properties. In this study, using multi-terminal measurements, we report high broadband photocurrent response ( R ) and external quantum efficiency (EQE) of few-atomic layered MoS 2 phototransistors fabricated on a SiO 2 dielectric substrate and encapsulated with a thin transparent polymer film of Cytop. The photocurrent response was measured using a white light source as well as a monochromatic light of wavelength λ = 400 nm–900 nm. We measured responsivity using a 2-terminal configuration as high as R = 1 × 10 3 A W -1 under white light illumination with an optical power P opt = 0.02 nW. The R value increased to 3.5 × 10 3 A W -1 when measured using a 4-terminal configuration. Using monochromatic light on the same device, the measured values of R were 10 3 and 6 × 10 3 A W -1 under illumination of λ = 400 nm when measured using 2- and 4-terminal methods, respectively. The highest EQE values obtained using λ = 400 nm were 10 5 % and 10 6 % measured using 2- and 4-terminal configurations, respectively. The wavelength dependent responsivity decreased from 400 nm to the near-IR region at 900 nm. The observed photoresponse, photocurrent–dark current ratio (PDCR), detectivity as a function of applied gate voltage, optical power, contact resistances and wavelength were measured and are discussed in detail. The observed responsivity is also thoroughly studied as a function of contact resistance of the device.

36 MATERIALS SCIENCE↗

Ultrathin alumina passivation for improved photoelectrochemical water oxidation catalysis of tin oxide sensitized by a phosphonate-functionalized perylene diimide first without, and then with, CoOy

Previously, a photoanode composed of nanostructured SnO 2 coated with the perylene diimide dye N,N'-bis(phosphonomethyl)-3,4,9,10-perylenediimide (PMPDI) plus photoelectrochemically deposited cobalt oxide (CoO y ) was shown to photoelectrochemically oxidize water at 31 ± 7% faradaic efficiency. A non-ideal part of that prior system is that the addition of the known CoO y water oxidation catalyst (WOC) resulted in a reduction of the total photocurrent rather than the anticipated increase, due to an increase in charge-carrier recombination. Herein, we show deposition of an ultrathin alumina overlayer applied by atomic layer deposition (ALD) on the SnO 2 /PMPDI photoanode can improve the photoactivity and catalytic activity of the system; the addition a ca. 1 nm-thick AlO x layer deposited on a 4000 nm (i.e., 4 micron) thick mesoporous anode system can and does have a positive, 2.5-fold improvement in the steady-state photocurrent with 29 ± 9% faradaic efficiency vs. the control anode without alumina passivation by reducing charge-carrier recombination. Moreover, ALD-deposited AlO x layer does help support the understanding of the “anti-catalysis” of co-depositing a CoO y WOC on the SnO 2 /PMPDI DS-PECs—specifically the picture of direct CoO y –SnO 2 contact-mediated recombination—but that AlO x layer was unable to improve the photocurrent in a net SnO 2 /PMPDI/AlO x (/CoO y ) system. We attribute the lack of a performance enhancement by CoOy WOC to incomplete coverage of each SnO 2 nanoparticle by the AlO x . Overall, we find the addition of an optimized ultrathin AlOx layer (0.6 nm thick; deposited at 85 °C) improves the SnO 2 /PMPDI/AlO x system's photoactivity by a factor of up to ca. 3-fold with reduced recombination. These results document that metal-oxide passivation by low-temperature ALD can be an effective strategy for improving the water oxidation performance of even nanostructured dye sensitized-photoelectrochemical cell.

36 MATERIALS SCIENCE↗

Voltage-dependent excitation dynamics in UV-absorbing organic photovoltaics with efficient charge transfer exciton emission

Intermolecular charge-transfer excitons play a central role in determining the performance of organic solar cells as their voltage-dependent formation, dissociation, and recombination dynamics contribute to photocurrent generation, radiative/nonradiative voltage losses, and photovoltaic fill factor. Here, we explore the properties of brightly-emitting wide energy gap (>2 eV) charge transfer excitons by measuring the voltage-dependent photoluminescence, photocurrent, and ultrafast pump–probe transient absorption spectra of organic solar cells employing five UV-absorbing donor molecules that differ only by the length of the oligophenylene or acene group at their core. We find that organic solar cells with a strong correlation between their voltage-dependent photocurrent and charge-transfer exciton photoluminescence have low photovoltaic fill factors as they require voltage to facilitate efficient charge-transfer exciton dissociation. In contrast, solar cells that are efficient can readily generate charges without an applied field and have a separate population of tightly-bound charge-transfer excitons that are responsible for emission. Furthermore, considering that the sum of all excitation loss rates (i.e., recombination and charge extraction) must be equal to the excitation generation rate in the steady state, these voltage-dependent data allow us to solve for the voltage-dependent fate of all excitations in the solar cells and estimate upper and lower bounds for geminate and non-geminate recombination, respectively.

14 SOLAR ENERGY↗

Room temperature infrared photoresponse of self assembled Ge/Si (001) quantum dots grown by molecular beam epitaxy

We report on the observation of intraband near infrared (approx3.1 mum) and mid infrared (approx6.2 mum) photocurrent response at room temperature using Ge/Si self-assembled quantum dots grown by molecular beam epitaxy. Due to the bimodal size distribution and SiGe intermixing, distinguishable photoluminescence transitions are observed at 10 K, below and above the optical band gap of bulk Ge. The observed redshift in photocurrent with increasing temperature has been explained by the excitonic electric field originated due to infrared excitation at low temperatures. A good correlation between the spectral photocurrent response and photoluminescence of the quantum dots has been established.

36 MATERIALS SCIENCE↗

Effect of charge compensation on the photoelectrochemical properties of Ho-doped SrTiO{sub 3} films

When Ho{sup 3+} ions are substituted at Sr{sup 2+} sites in SrTiO{sub 3} (STO), the excess positive charges are compensated via three complementary routes: (1) strontium vacancies, (2) titanium vacancies, and (3) conduction electrons. In this study, we show that the photoelectrochemical properties of Ho-doped STO films are dependent on the charge compensation mechanisms. The compensation mechanism via the titanium vacancies exhibits the highest photocurrent density, which is 1.7 times higher than that of the pure STO sample. Based on the measured dielectric properties and electrochemical impedance spectroscopy data, we propose that the enhanced dielectric constant of the films can enlarge the width of the space charge region at the film/liquid interface, which eventually leads to the increase of the photocurrent density. Further enhancement of photocurrent density is obtained in the samples decorated with appropriate amounts of Pt nanoparticles, showing the advantage of composites for achieving the efficient photoelectrochemical property.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Photoconductivity of germanium tin alloys grown by molecular beam epitaxy

Photocurrent spectroscopy was used to measure the infrared absorption of germanium-tin alloys grown by molecular beam epitaxy. To study dependence on Sn composition, the photocurrent was measured at 100 K on alloys of Ge{sub 1-x}Sn{sub x} with atomic percentages of Sn up to 9.8%. The optical absorption coefficient was calculated from the photocurrent, and it was found that the absorption edge and extracted bandgap energy decreased with increasing Sn content. For all Ge{sub 1-x}Sn{sub x} samples, a fundamental bandgap below that of bulk Ge was observed, and a bandgap energy as low as 0.624 eV was found for a Sn percentage of 9.8% at 100 K.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

The operation principle of the well in quantum dot stack infrared photodetector

The well in the quantum dot stack infrared photodetector (WD-QDIP) is proposed which can be operated at high temperature ∼230 K. The operation principle of this device is investigated, including the carrier transport and the enhancement in the photocurrent. The WD-QDIPs with different well numbers are fabricated to study the mechanisms. It is realized that the carrier transport from the emitter to the collector in traditional quantum dot infrared photodetectors consists of two channels deduced from current-voltage characteristics and dark current activation energy at different temperatures. At temperatures below 77 K, the current transports through the InAs quantum dot channel, whereas at temperatures higher than 77 K, the current is dominated by the GaAs leakage channel. In addition, the non-equilibrium situation at low temperatures is also observed owing to the presence of photovoltaic phenomenon. The carrier distribution inside the QDs is simulated to investigate the reasons for the increase of photocurrent. Based on the simulation and the photocurrent response, the hot carrier (electron) scattering effect by the insertion of a quantum well layer is inferred as the most probable reason that lead to the enhancement of the response and regarded as the key factor to achieve high- temperature operation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Impact of transparent electrode on photoresponse of ZnO-based phototransistor

ZnO-based photo-thin film transistors with enhanced photoresponse were developed using transparent conductive oxide contacts. Changing the electrode from opaque Mo to transparent In-Zn-O increases the photocurrent by five orders of magnitude. By changing the opacity of each source and drain electrode, we could observe how the photoresponse is affected. We deduce that the photocurrent generation mechanism is based on an energy band change due to the photon irradiation. More importantly, we reveal that the photocurrent is determined by the energy barrier of injected electrons at the interface between the source electrode and the active layer.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Photovoltaic effect of lead-free (Na{sub 0.82}K{sub 0.18}){sub 0.5}Bi{sub 4.5}Ti{sub 4}O{sub 15} ferroelectric thin film using Pt and indium tin oxide top electrodes

We have grown a Bi-layer structure (Na{sub 0.82}K{sub 0.18}){sub 0.5}Bi{sub 4.5}Ti{sub 4}O{sub 15} (NKBiT) ferroelectric thin film on Pt(111)/TiO{sub 2}/SiO{sub 2}/Si(100) substrate by using the chemical solution deposition method and deposited two kinds of thin Pt and indium tin oxide (ITO) top electrodes. The photovoltaic behaviors of Pt/NKBiT/Pt and ITO/NKBit/Pt capacitors were investigated over the wavelength range of 300–500 nm. When NKBiT thin film is illuminated by the corresponding wavelength of the film's energy band gap (E{sub g}), a photocurrent is generated due to the Schottky barrier between electrode and film, and an internal electric field is originated by the depolarization field. The maximum photocurrent density and power conversion efficiency of the ITO/NKBiT/Pt capacitor in the poled-up state are obtained as 45.75 nA/cm{sup 2} and 0.035%, respectively, at 352 nm. The photocurrent density and power conversion efficiency of the ITO/NKBiT/Pt capacitor increased to 3.5 times higher than that of the Pt/NKBiT/Pt capacitor.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Oxygen vacancies induced switchable and nonswitchable photovoltaic effects in Ag/Bi{sub 0.9}La{sub 0.1}FeO{sub 3} /La{sub 0.7}Sr{sub 0.3}MnO{sub 3} sandwiched capacitors

The short circuit photocurrent (I{sub sc}) was found to be strongly dependent on the oxygen vacancies (V{sub Os}) distribution in Ag/Bi{sub 0.9}La{sub 0.1}FeO{sub 3}/La{sub 0.7}Sr{sub 0.3}MnO{sub 3} heterostructures. In order to manipulate the V{sub Os} accumulated at either the Ag/Bi{sub 0.9}La{sub 0.1}FeO{sub 3} or the Bi{sub 0.9}La{sub 0.1}FeO{sub 3}/La{sub 0.7}Sr{sub 0.3}MnO{sub 3} interface by pulse voltages, switchable or nonswitchable photocurrent can be observed without or with changing the polarization direction. The sign of photocurrent could be independent of the direction of polarization when the variation of diffusion current and the modulation of the Schottky barrier at the Ag/Bi{sub 0.9}La{sub 0.1}FeO{sub 3} interface induced by oxygen vacancies are large enough to offset those induced by polarization. Our work provides deep insights into the nature of photovoltaic effects in ferroelectric films, and will facilitate the advanced design of switchable devices combining spintronic, electronic, and optical functionalities.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Excess carrier generation in femtosecond-laser processed sulfur doped silicon by means of sub-bandgap illumination

With Fourier-transform photocurrent spectroscopy and spectral response measurements, we show that silicon doped with sulfur by femtosecond laser irradiation generates excess carriers, when illuminated with infrared light above 1100 nm. Three distinct sub-bandgap photocurrent features are observed. Their onset energies are in good agreement with the known sulfur levels S{sup +}, S{sup 0}, and S{sub 2}{sup 0}. The excess carriers are separated by a pn-junction to form a significant photocurrent. Therefore, this material likely demonstrates the impurity band photovoltaic effect.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Study on negative incident photon-to-electron conversion efficiency of quantum dot-sensitized solar cells

Recently, negative signals are frequently observed during the measuring process of monochromatic incident photon-to-electron conversion efficiency (IPCE) for sensitized solar cells by DC method. This phenomenon is confusing and hindering the reasonable evaluation of solar cells. Here, cause of negative IPCE values is studied by taking quantum dot-sensitized solar cell (QDSC) as an example, and the accurate measurement method to avoid the negative value is suggested. The negative background signals of QDSC without illumination are found the direct cause of the negative IPCE values by DC method. Ambient noise, significant capacitance characteristics, and uncontrolled electrochemical reaction all can lead to the negative background signals. When the photocurrent response of device under monochromatic light illumination is relatively weak, the actual photocurrent signals will be covered by the negative background signals and the resulting IPCE values will appear negative. To improve the signal-to-noise ratio, quasi-AC method is proposed for IPCE measurement of solar cells with weak photocurrent response based on the idea of replacing the absolute values by the relative values.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗