Gate Controlled Excitonic Emission in Quantum Dot Thin Films.

Formation of charged trions is detrimental to the luminescence quantum efficiency of colloidal quantum dot (QD) thin films as they predominantly undergo nonradiative recombination. In this regard, control of charged trion formation is of interest for both fundamental characterization of the quasi-particles and performance optimization. Using CdSe/CdS QDs as a prototypical material system, here we demonstrate a metal-oxide-semiconductor capacitor based on QD thin films for studying the background charge effect on the luminescence efficiency and lifetime. The concentration ratio of the charged and neutral quasiparticles in the QDs is reversibly controlled by applying a gate voltage, while simultaneous steady-state and time-resolved photoluminescence measurements are performed. Notably, the photoluminescence intensity is modulated by up to 2 orders of magnitude with a corresponding change in the effective lifetime. In addition, chip-scale modulation of brightness is demonstrated, where the photoluminescence is effectively turned on and off by the gate, highlighting potential applications in voltage-controlled electrochromics.

Highly multicolored light-emitting arrays for compressive spectroscopy.

Miniaturized, multicolored light-emitting device arrays are promising for applications in sensing, imaging, computing, and more, but the range of emission colors achievable by a conventional light-emitting diode is limited by material or device constraints. In this work, we demonstrate a highly multicolored light-emitting array with 49 different, individually addressable colors on a single chip. The array consists of pulsed-driven metal-oxide-semiconductor capacitors, which generate electroluminescence from microdispensed materials spanning a diverse range of colors and spectral shapes, enabling facile generation of arbitrary light spectra across a broad wavelength range (400 to 1400 nm). When combined with compressive reconstruction algorithms, these arrays can be used to perform spectroscopic measurements in a compact manner without diffractive optics. As an example, we demonstrate microscale spectral imaging of samples using a multiplexed electroluminescent array in conjunction with a monochrome camera.

Anomalous thickness dependence of photoluminescence quantum yield in black phosphorous.

Black phosphorus has emerged as a unique optoelectronic material, exhibiting tunable and high device performance from mid-infrared to visible wavelengths. Understanding the photophysics of this system is of interest to further advance device technologies based on it. Here we report the thickness dependence of the photoluminescence quantum yield at room temperature in black phosphorus while measuring the various radiative and non-radiative recombination rates. As the thickness decreases from bulk to ~4 nm, a drop in the photoluminescence quantum yield is initially observed due to enhanced surface carrier recombination, followed by an unexpectedly sharp increase in photoluminescence quantum yield with further thickness scaling, with an average value of ~30% for monolayers. This trend arises from the free-carrier to excitonic transition in black phosphorus thin films, and differs from the behaviour of conventional semiconductors, where photoluminescence quantum yield monotonically deteriorates with decreasing thickness. Furthermore, we find that the surface carrier recombination velocity of black phosphorus is two orders of magnitude lower than the lowest value reported in the literature for any semiconductor with or without passivation; this is due to the presence of self-terminated surface bonds in black phosphorus.

Deep ultraviolet spontaneous emission enhanced by layer dependent black phosphorus plasmonics.

Although graphene has been the primary material of interest recently for spontaneous emission engineering through the Purcell effect, it features isotropic and thickness-independent optical properties. In contrast, the optical properties of black Phosphorus (BP) are in-plane anisotropic; which supports plasmonic modes and are thickness-dependent, offering an additional degree of freedom for control. Here we investigate how the anisotropy and thickness of BP affect spontaneous emission from a Hydrogenic emitter. We find that the spontaneous emission enhancement rate i.e. Purcell factor (PF) depends on emitter orientation, and PF at a particular frequency and distance can be controlled by BP thickness. At lower frequencies, PF increases with increasing thickness due to infrared (IR) plasmons, which then enhances visible and UV far-field spectra, even at energies greater than 10 eV. By leveraging the thickness and distance-dependent PF, deep UV emission can be switched between 103 nm or 122 nm wavelength from a Hydrogenic emitter. Additionally, we find that doping can significantly tune the PF near BP and this alteration depends on the thickness of the BP. Our work shows that BP is a promising platform for studying strong plasmon-induced light-matter interactions tunable by varying doping levels, emitter orientation, and thickness.

Efficiency Roll-Off Free Electroluminescence from Monolayer WSe2.

Exciton-exciton annihilation (EEA) is a nonradiative process commonly observed in excitonic materials at high exciton densities. Like Auger recombination, EEA degrades luminescence efficiency at high exciton densities and causes efficiency roll-off in light-emitting devices. Near-unity photoluminescence quantum yield has been demonstrated in transition metal dichalcogenides (TMDCs) at all exciton densities with optimal band structure modification mediated by strain. Although the recombination pathways in TMDCs are well understood, the practical application of light-emitting devices has been challenging. Here, we demonstrate a roll-off free electroluminescence (EL) device composed of TMDC monolayers tunable by strain. We show a 2 orders of magnitude EL enhancement from the WSe2 monolayer by applying a small strain of 0.5%. We attain an internal quantum efficiency of 8% at all injection rates. Finally, we demonstrate transient EL turn-on voltages as small as the band gap. Our approach will contribute to practical applications of roll-off free optoelectronic devices based on excitonic materials.

Enhanced Neutral Exciton Diffusion in Monolayer WS2 by Exciton-Exciton Annihilation.

Dominant recombination pathways in monolayer transition metal dichalcogenides (TMDCs) depend primarily on background carrier concentration, generation rate, and applied strain. Charged excitons formed in the presence of background carriers mainly recombine nonradiatively. Neutral excitons recombine completely radiatively at low generation rates, but experience nonradiative exciton-exciton annihilation (EEA) at high generation rates. Strain can suppress EEA, resulting in near-unity photoluminescence quantum yield (PL QY) at all exciton densities. Although exciton diffusion is the primary channel of energy transport in excitonic materials and a critical optoelectronic design consideration, the combined effects of these factors on exciton diffusion are not clearly understood. In this work, we decouple the diffusion of neutral and charged excitons with chemical counterdoping and explore the effect of strain and generation rate on exciton diffusion. According to the standard semiconductor paradigm, a shorter carrier recombination lifetime should lead to a smaller diffusion length. Surprisingly, we find that increasing generation rate shortens the exciton lifetime but increases the diffusion length in unstrained monolayers of TMDCs. When we suppress EEA by strain, both lifetime and diffusion length become independent of generation rate. During EEA one exciton nonradiatively recombines and kinetically energizes another exciton, which then diffuses fast. Our results probe concentration-dependent diffusion of pure neutral excitons by counterdoping and elucidate how strain controls exciton transport and many-body interactions in TMDC monolayers.

Bright Mid-Wave Infrared Resonant-Cavity Light-Emitting Diodes Based on Black Phosphorus.

The mid-wave infrared (MWIR) wavelength range plays a central role in a variety of applications, including optical gas sensing, industrial process control, spectroscopy, and infrared (IR) countermeasures. Among the MWIR light sources, light-emitting diodes (LEDs) have the advantages of simple design, room-temperature operation, and low cost. Owing to the low Auger recombination at high carrier densities and direct bandgap of black phosphorus (bP), it can serve as a high quantum efficiency emitting layer in LEDs. In this work, we demonstrate bP-LEDs exhibiting high external quantum efficiencies and wall-plug efficiencies of up to 4.43 and 1.78%, respectively. This is achieved by integrating the device with an Al2O3/Au optical cavity, which enhances the emission efficiency, and a thin transparent conducing oxide [indium tin oxide (ITO)] layer, which reduces the parasitic resistance, both resulting in order of magnitude improvements to performance.

Engineering Exciton Recombination Pathways in Bilayer WSe2 for Bright Luminescence.

Exciton-exciton annihilation (EEA) in counterdoped monolayer transition metal dichalcogenides (TMDCs) can be suppressed by favorably changing the band structure with strain. The photoluminescence (PL) quantum yield (QY) monotonically approaches unity with strain at all generation rates. In contrast, here in bilayers (2L) of tungsten diselenide (WSe2) we observe a nonmonotonic change in EEA rate at high generation rates accompanied by a drastic enhancement in their PL QY at low generation rates. EEA is suppressed at both 0% and 1% strain, but activated at intermediate strains. We explain our observation through the indirect to direct transition in 2L WSe2 under uniaxial tensile strain. By strain and electrostatic counterdoping, we attain ∼50% PL QY at all generation rates in 2L WSe2, originally an indirect semiconductor. We demonstrate transient electroluminescence from 2L WSe2 with ∼1.5% internal quantum efficiency for a broad range of carrier densities by applying strain, which is ∼50 times higher than without strain. The present results elucidate the complete optoelectronic photophysics where indirect and direct excitons are simultaneously present and expedite exciton engineering in a TMDC multilayer beyond indirect-direct bandgap transition.

Inhibited nonradiative decay at all exciton densities in monolayer semiconductors.

Most optoelectronic devices operate at high photocarrier densities, where all semiconductors suffer from enhanced nonradiative recombination. Nonradiative processes proportionately reduce photoluminescence (PL) quantum yield (QY), a performance metric that directly dictates the maximum device efficiency. Although transition metal dichalcogenide (TMDC) monolayers exhibit near-unity PL QY at low exciton densities, nonradiative exciton-exciton annihilation (EEA) enhanced by van-Hove singularity (VHS) rapidly degrades their PL QY at high exciton densities and limits their utility in practical applications. Here, by applying small mechanical strain (less than 1%), we circumvented VHS resonance and markedly suppressed EEA in monolayer TMDCs, resulting in near-unity PL QY at all exciton densities despite the presence of a high native defect density. Our findings can enable light-emitting devices that retain high efficiency at all brightness levels.

Actively variable-spectrum optoelectronics with black phosphorus.

Room-temperature optoelectronic devices that operate at short-wavelength and mid-wavelength infrared ranges (one to eight micrometres) can be used for numerous applications1-5. To achieve the range of operating wavelengths needed for a given application, a combination of materials with different bandgaps (for example, superlattices or heterostructures)6,7 or variations in the composition of semiconductor alloys during growth8,9 are used. However, these materials are complex to fabricate, and the operating range is fixed after fabrication. Although wide-range, active and reversible tunability of the operating wavelengths in optoelectronic devices after fabrication is a highly desirable feature, no such platform has been yet developed. Here we demonstrate high-performance room-temperature infrared optoelectronics with actively variable spectra by presenting black phosphorus as an ideal candidate. Enabled by the highly strain-sensitive nature of its bandgap, which varies from 0.22 to 0.53 electronvolts, we show a continuous and reversible tuning of the operating wavelengths in light-emitting diodes and photodetectors composed of black phosphorus. Furthermore, we leverage this platform to demonstrate multiplexed nondispersive infrared gas sensing, whereby multiple gases (for example, carbon dioxide, methane and water vapour) are detected using a single light source. With its active spectral tunability while also retaining high performance, our work bridges a technological gap, presenting a potential way of meeting different requirements for emission and detection spectra in optoelectronic applications.

Universal Inverse Scaling of Exciton-Exciton Annihilation Coefficient with Exciton Lifetime.

Be it for essential everyday applications such as bright light-emitting devices or to achieve Bose-Einstein condensation, materials in which high densities of excitons recombine radiatively are crucially important. However, in all excitonic materials, exciton-exciton annihilation (EEA) becomes the dominant loss mechanism at high densities. Typically, a macroscopic parameter named EEA coefficient (CEEA) is used to compare EEA rates between materials at the same density; higher CEEA implies higher EEA rate. Here, we find that the reported values of CEEA for 140 different materials is inversely related to the single-exciton lifetime. Since during EEA one exciton must relax to ground state, CEEA is proportional to the single-exciton recombination rate. This leads to the counterintuitive observation that the exciton density at which EEA starts to dominate is higher in a material with larger CEEA. These results broaden our understanding of EEA across different material systems and provide a vantage point for future excitonic materials and devices.

Neutral Exciton Diffusion in Monolayer MoS2.

Monolayer transition metal dichalcogenides (TMDCs) are promising materials for next generation optoelectronic devices. The exciton diffusion length is a critical parameter that reflects the quality of exciton transport in monolayer TMDCs and limits the performance of many excitonic devices. Although diffusion lengths of a few hundred nanometers have been reported in the literature for as-exfoliated monolayers, these measurements are convoluted by neutral and charged excitons (trions) that coexist at room temperature due to natural background doping. Untangling the diffusion of neutral excitons and trions is paramount to understand the fundamental limits and potential of new optoelectronic device architectures made possible using TMDCs. In this work, we measure the diffusion lengths of neutral excitons and trions in monolayer MoS2 by tuning the background carrier concentration using a gate voltage and utilizing both steady state and transient spectroscopy. We observe diffusion lengths of 1.5 µm and 300 nm for neutral excitons and trions, respectively, at an optical power density of 0.6 W cm-2.

Electrical suppression of all nonradiative recombination pathways in monolayer semiconductors.

Defects in conventional semiconductors substantially lower the photoluminescence (PL) quantum yield (QY), a key metric of optoelectronic performance that directly dictates the maximum device efficiency. Two-dimensional transition-metal dichalcogenides (TMDCs), such as monolayer MoS2, often exhibit low PL QY for as-processed samples, which has typically been attributed to a large native defect density. We show that the PL QY of as-processed MoS2 and WS2 monolayers reaches near-unity when they are made intrinsic through electrostatic doping, without any chemical passivation. Surprisingly, neutral exciton recombination is entirely radiative even in the presence of a high native defect density. This finding enables TMDC monolayers for optoelectronic device applications as the stringent requirement of low defect density is eased.

A Robust Heart Rate Monitoring Scheme Using Photoplethysmographic Signals Corrupted by Intense Motion Artifacts.

GOAL: Although photoplethysmographic (PPG) signals can monitor heart rate (HR) quite conveniently in hospital environments, trying to incorporate them during fitness programs poses a great challenge, since in these cases, the signals are heavily corrupted by motion artifacts. METHODS: In this paper, we present a novel signal processing framework which utilizes two channel PPG signals and estimates HR in two stages. The first stage eliminates any chances of a runaway error by resorting to an absolute criterion condition based on ensemble empirical mode decomposition. This stage enables the algorithm to depend very little on the previously estimated HR values and to discard the need of an initial resting phase. The second stage, on the other hand, increases the algorithm's robustness against offtrack errors by using recursive least squares filters complemented with an additional novel technique, namely time-domain extraction. RESULTS: Using this framework, an average absolute error of 1.02 beat per minute (BPM) and standard deviation of 1.79 BPM are recorded for 12 subjects performing a run with peak velocities reaching as high as 15 km/h. CONCLUSION: The performance of this algorithm is found to be better than the other recently reported algorithms in this field such as TROIKA and JOSS. SIGNIFICANCE: This method is expected to greatly facilitate the presently available wearable gadgets in HR computation during various physical activities.