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Sn-doped indium oxide (ITO) semiconductor nano-films are fabricated by plasma-enhanced atomic layer deposition using trimethylindium (TMIn), tetrakis(dimethylamino)tin (TDMASn), and O2plasma as the sources of In, Sn and O, respectively. A shared temperature window of 150 °C- 200 °C is observed for the deposition of ITO nano-films. The introduction of Sn into indium oxide is found to increase the concentration of oxygen into the ITO films and inhibit crystallization. Furthermore, two oxidation states are observed for In and Sn, respectively. With the increment of interfaces of In-O/Sn-O in the ITO films, the relative percentage of In3+ions increases and that of Sn4+decreases, which is generated by interfacial competing reactions. By optimizing the channel component, the In0.77Sn0.23O1.11thin-film transistors (TFTs) demonstrate high performance, includingµFEof 52.7 cm2V-1s-1, and a highION/IOFFof â¼5 × 109. Moreover, the devices show excellent positive bias temperature stress stability at 3 MV cm-1and 85 °C, i.e. a minimalVthshift of 0.017 V after 4 ks stress. This work highlights the successful application of ITO semiconductor nano-films by ALD for TFTs.
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Hf0.5Zr0.5O2(HZO) has drawn great attention owing to its excellent ferroelectricity, sub-10 nm scalability, and CMOS compatibility. With regard to increasingly restrict thermal budget and power consumption, conventional HZO films need further optimization to meet these demands. Here, we propose a middle layer (ML) strategy aiming to enhance ferroelectricity and inhibit wake-up effect of ferroelectric (FE) capacitors compatible with back-end of line (BEOL) under the low operating electric field. ZrO2, HfO2, and Al2O3were integrated into HZO film as different MLs. Among them, the device with ZrO2ML achieves the excellent double remnant polarization (2Pr) of 41.7 µC/cm2under the operating electric field of 2 MV/cm. Moreover, ultralow wake-up ratios of around 0.08 and 0.05 were observed under 2 MV/cm and 3 MV/cm, respectively. Additionally, the FE capacitor with ZrO2ML demonstrated an enhanced reliability characterizations, including a stable 2Pr of 40.7 µC/cm2after 4.3×109cycles. This work provides the perspective to optimize both the ferroelectricity and reliability, while maintains the ultralow wake-up ratio in HfO2-based ferroelectric through middle layer engineering. .
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Ferroelectric field effect transistor (FeFET) memories with hafnium zirconium oxide (HZO) ferroelectric gate dielectric and ultrathin InOxchannel exhibit promising applicability in monolithic three-dimensional (M3D) integrated chips. However, the inferior stability of the devices severely limits their applications. In this work, we studied the effect of single cycle of atomic-layer-deposited Al-O bonds repeatedly embedded into an ultrathin InOxchannel (â¼2.8 nm) on the Hf0.45Zr0.55OxFeFET memory performance. Compared to the pure InOxchannel, three cycles of Al-O bonds modified InOxchannel (IAO-3) generates a much larger memory window (i.e. drain current ratio between the programmed and erased devices) under the same program conditions (+5.5 V/500 ns), especially after post-annealing at 325 °C for 180 s in O2(1238 versus 317). Meanwhile, the annealed IAO-3 FeFET memory also shows quite stable data retention up to 104s, and much more robust program/erase stabilities till 105cycles. This is because the modification of strong Al-O bonds stabilizes the oxygen vacancies and reduces the bulk trap density in the channel. Furthermore, it is indicated that the program and erase efficiencies increase gradually with reducing the channel length of the memory device. By demonstrating markedly improved performance of the HZO FeFET memory with the ultrathin IAO-3 channel, this work provides a promising device for M3D integratable logic and memory convergent systems.
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Halide perovskites are promising photoactive materials for filter-free color-imaging sensors owing to their outstanding optoelectronic properties, tunable bandgaps, and suitability for large-scale fabrication. However, producing patterned perovskite films of sufficiently high quality for such applications poses a challenge for existing fabrication methods: using solution processes to prepare patterned perovskite films is complicated, while evaporation methods often result in perovskite photodetectors with limited performance. In this paper, the authors report the development of an improved evaporation method in which substrates are treated with a brominated (3-aminopropyl) triethoxysilane self-assembled monolayer to improve the properties of the patterned perovskite films. The resulting perovskite photodetectors exhibit significantly enhanced photosensitivity and long-term stability (exceeding 100 days). Additionally, the polymer substrates facilitate device flexibility. Finally, perovskites comprising three different halide components, each with a different bandgap, are integrated into a device array using the developed evaporation technology, yielding sensors that enable the discrimination of red, green, and blue colors. Thus, the flexible photosensor arrays can generate colorful images closely resembling perceived patterns, demonstrating reliable color imaging. Therefore, this study successfully demonstrates filter-free color-imaging by integrating high-performance patterned and multicomponent perovskite photodetectors, highlighting the potential of such detectors for advanced optoelectronic applications, including hyperspectral imaging.
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The electronic-photonic convergent systems can overcome the data transmission bottleneck for microchips by enabling processor and memory chips with high-bandwidth optical input/output. However, current silicon-based electronic-photonic systems require various functional devices/components to convert high-bandwidth optical signals into electrical ones, thus making further integrations of sophisticated systems rather difficult. Here, we demonstrate thin-film transistor-based photoelectric memories employing CsPbBr3/CsPbI3 blend perovskite quantum dots (PQDs) as a floating gate, and multilevel memory cells are achieved under programming and erasing modes, respectively, by imputing high-bandwidth optical signals. For different bandwidth light input (i.e. 500-550, 575-650 and 675-750 nm) with the same intensity, three levels of programming window (i.e. 3.7, 1.9 and 0.8 V) and erasing window (i.e. -1.9, -0.6 and -0.1 V) are obtained under electrical pulses, respectively. This is because the blend PQDs have two different bandgaps, and different amounts of photo-generated carriers can be produced for different wavelength optical inputs. It is noticed that the 675-750 nm light inputs have no effects on both programming and erasing windows because of no photo-carriers generation. Four memory states are demonstrated, showing enough large gaps (1.12-5.61 V) between each other, good data retention and programming/erasing endurance. By inputting different optical signals, different memory states can be switched easily. Therefore, this work directly demonstrates high-bandwidth light inputting multilevel memory cells for novel electronic-photonic systems.
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To construct an artificial intelligence system with high efficient information integration and computing capability like the human brain, it is necessary to realize the biological neurotransmission and information processing in artificial neural network (ANN), rather than a single electronic synapse as most reports. Because the power consumption of single synaptic event is â¼10 fJ in biology, designing an intelligent memristors-based 3D ANN with energy consumption lower than femtojoule-level (e.g., attojoule-level) and faster operating speed than millisecond-level makes it possible for constructing a higher energy efficient and higher speed computing system than the human brain. In this paper, a flexible 3D crossbar memristor array is presented, exhibiting the multilevel information transmission functionality with the power consumption of 4.28 aJ and the response speed of 50 ns per synaptic event. This work is a significant step toward the development of an ultrahigh efficient and ultrahigh-speed wearable 3D neuromorphic computing system.
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Surface-plasmon mediated photoluminescence emission enhancement has been investigated for ZnO nanowire (NW)/Pt nanoparticle (NP) nanostructures by inserting an Al2O3 spacer layer. The thickness of the Al2O3 spacer layer and of the Pt NPs capped on the ZnO NWs are well controlled by atomic layer deposition. It is found that the photoluminescence property of the ZnO NW/Al2O3/Pt hybrid structure is highly tunable with respect to the thickness of the inserted Al2O3 spacer layer. The highest enhancement (â¼14 times) of the near band emission of ZnO NWs is obtained with an optimized Al2O3 spacer layer thickness of 10 nm leading to a ultraviolet-visible emission ratio of 271.2 compared to 18.8 for bare ZnO NWs. The enhancement of emission is influenced by a Förster-type non-radiative energy transfer process of the exciton energy from ZnO NWs to Pt NPs as well as the coupling effect between excitons of ZnO NWs and surface plasmons of Pt NPs. The highly versatile and tunable photoluminescence properties of Pt-coated ZnO NWs achieved by introducing an Al2O3 spacer layer demonstrate their potential application in highly efficient optoelectronic devices.
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The effects of shell thickness and rapid thermal annealing on photoluminescence properties of one-dimensional ZnO/ZrO2 core/shell nanowires (NWs) are studied in this work. The ZnO/ZrO2 core/shell structures were synthesized by coating thin ZrO2 layers on the surface of ZnO NWs using atomic layer deposition. The morphological and structural characterization studies reveal that the ZrO2 shells have a polycrystalline structure, which are uniformly and conformally coated on the high quality single-crystal ZnO NWs. As compared with bare ZnO NWs, the ZnO/ZrO2 core/shell structures show a remarkable and continuous enhancement of ultraviolet (UV) emission in intensity with increasing ZrO2 shell thickness up to 10 nm. The great improvement mechanism of the UV emission arises from the surface passivation and the efficient carrier confinement effect of the type-I core/shell system. Moreover, it is observed that the UV emission of ZnO/ZrO2 core/shell structures after thermal annealing increases with increasing annealing temperature. The dominant surface exciton (SX) emission in the bare ZnO NWs and the ZnO/ZrO2 core/shell nanostructures has been detected in the low temperature photoluminescence spectra. A blue shift of the NBE emission peak as well as the varied decay rate of the SX emission intensity are also found in the ZnO NWs after the growth of ZrO2 shells and further thermal treatment. Our results suggest that the ZnO/ZrO2 core/shell nanostructures could be widely implemented in the optical and electronic devices in the future.
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Effects of ZnO seed layer annealing temperature on the characteristics of the n-ZnO nanowires/Al(2)O(3)/p-Si heterojunction are investigated. Well-aligned ZnO nanowires (NWs) are grown through a simple hydrothermal method. Both the insertion of Al(2)O(3) buffer layer and the annealing treatment of ZnO seed layer are advantageous for the growth of ZnO NWs. This leads to a relatively high rectification ratio of up to 7.8 × 10(3) at ± 4.0 V in ZnO NWs/Al(2)O(3)/p-Si heterojunction photodetectors. The photoelectrical property of n-ZnO/p-Si photodetectors with an enhanced UV/dark current ratio as high as 30 under a reverse bias of 4.0 V is obtained.
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The n-ZnO/p-Si heterojunction with an ultrathin Al2O3 buffer layer was prepared by atomic layer deposition. X-ray diffraction revealed that the crystalline quality of (100)-oriented ZnO films was improved with an Al2O3 buffer layer. The n-ZnO/p-Si heterojunction with 5 nm inserted Al2O3 layer shows the best electrical characteristics, with a dark current of 0.5 µA at a reverse bias of -2 V and increasing the photo-to-dark current ratio effectively by 8 times. These results demonstrated that Al2O3 buffer layer with optimized thickness exhibits significant advantages in enhancing the crystal quality of ZnO film and improving the photoelectrical properties of n-ZnO/p-Si photodetectors.
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Filter-free wavelength-selective photodetectors have garnered significant attention due to the growing demand for smart sensors, artificial intelligence, the Internet of Everything, and so forth. However, the challenges associated with large-scale preparation and compatibility with complementary metal-oxide-semiconductor (CMOS) technology limit their wide-ranging applications. In this work, we address the challenges by constructing vertically stacked graded-band-gap zinc-tin oxide (ZTO) thin-film transistors (TFTs) specifically designed for wavelength-selective photodetection. The ZTO thin films with various band gaps are fabricated via atomic layer deposition (ALD) by varying the ALD cycle ratios of zinc oxide (ZnO) and SnO2. The ZTO film with a small Sn ratio exhibits a decreased band gap, and the resultant TFT shows a degraded performance, which can be attributed to the Sn4+ dopant introducing a series of deep-state energy levels in the ZnO band gap. As the ratio of Sn increases further, the band gap of the ZTO also increases, and the mobility of the ZTO TFT increases up to 30 cm2/V s, with a positive shift of the threshold voltage. The photodetectors employing ZTO thin films with distinct band gaps show different spectral responsivities. Then, vertically stacked ZTO (S-ZTO) thin films, with gradient band gaps increasing from the bottom to the top, have been successfully deposited using consecutive ALD technology. The S-ZTO TFT shows decent performance with a mobility of 18.4 cm2/V s, a threshold voltage of 0.5 V, an on-off current ratio higher than 107, and excellent stability under ambient conditions. The resultant S-ZTO TFT also exhibits obviously distinct photoresponses to light at different wavelength ranges. Furthermore, a device array of S-ZTO TFTs demonstrates color imaging by precisely reconstructing patterned illuminations with different wavelengths. Therefore, this work provides CMOS-compatible and structure-compact wavelength-selective photodetectors for advanced and integrable optoelectronic applications.
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Miniaturized spectrometers have attracted much attention due to their capability to detect spectral information within a small size. However, such technology still faces challenges including large-scale preparation and performance repeatability. In this work, we overcome these challenges by demonstrating a microspectrometer constructed with a series of pixelized graded-bandgap perovskite photodetectors fabricated with inkjet printing. High-quality perovskite films with minimal pinholes and large grains are deposited by optimizing printing conditions including substrate temperature and surface modification. The resulting perovskite photodetectors show decent photosensing performance, and the different photodetectors based on perovskite films with different bandgaps exhibit various spectral responsivities with different cutoff wavelength edges. Microspectrometers are then constructed with the array of the pixelized graded-bandgap perovskite photodetectors, and incident spectra are algorithmically reconstructed by combining their output currents. The reconstruction performance of the miniaturized spectrometer is evaluated by comparing the results to the spectral curve measured with a commercial bulky spectrometer, indicating a reliable spectral reconstruction with a resolution of around 10 nm. More significantly, the miniaturized spectrometers are successfully fabricated on polymer substrates, and they demonstrate excellent mechanical flexibility. Therefore, this work provides a flexible miniaturized spectrometer with large-scale fabricability, which is promising for emerging applications including wearable devices, hyperspectral imaging, and internet of things.
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Concurrently achieving high energy storage density (ESD) and efficiency has always been a big challenge for electrostatic energy storage capacitors. In this study, we successfully fabricate high-performance energy storage capacitors by using antiferroelectric (AFE) Al-doped Hf0.25Zr0.75O2 (HfZrO:Al) dielectrics together with an ultrathin (1 nm) Hf0.5Zr0.5O2 underlying layer. By optimizing the Al concentration in the AFE layer with the help of accurate controllability of the atomic layer deposition technique, an ultrahigh ESD of 81.4 J cm-3 and a perfect energy storage efficiency (ESE) of 82.9% are simultaneously achieved for the first time in the case of the Al/(Hf + Zr) ratio of 1/16. Meanwhile, both the ESD and ESE exhibit excellent electric field cycling endurance within 109 cycles under 5~5.5 MV cm-1, and robust thermal stability up to 200 °C. Thus, the fabricated capacitor is very promising for on-chip energy storage applications due to favorable integratability with the standard complementary metal-oxide-semiconductor (CMOS) process.
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Function convergence of gas sensing and neuromorphic computing is attracting much research attention due to the promising potential in electronic olfactory, artificial intelligence, and internet of everything systems. However, the current neuromorphic gas-sensing systems are either realized via integration of gas detectors and neuromorphic devices or operating with three-terminal synaptic transistors at high voltages, leading to a rather high system complexity or power consumption. Herein, gas-modulated synaptic diodes with lateral structures are developed to converge sensing, processing, and storage functions into a single device. The lateral synaptic diode is based on a p-n junction of an organic semiconductor (OSC) and amorphous In-Ga-Zn-O, in which the upper OSC layer can directly interact with the gas molecules in the atmosphere. Typical synaptic behaviors triggered by ammonia, including inhibitory postsynaptic current and paired-pulse depression, are successfully demonstrated. Meanwhile, a low power consumption of 6.3 pJ per synaptic event has been achieved, which benefits from the simple device structure, the decent chemosensitivity of the OSC, and the low operation voltage. A simulated ammonia analysis in human exhaled breath is further conducted to explore the practical application of the synaptic diode. Therefore, this work provides a gas-modulated synaptic diode for circuit-compact and power-efficient artificial olfactory systems.
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Electronic-Photonic integrated systems have attracted intensive attention in addressing the explosively increasing data-processing issue in the post-Moore era. However, the tremendous size difference between basic electronic and photonic units poses challenges for the further deep convergence of optoelectronic microprocessors. Here, we report a floating-gate transistor fabricated with complementary metal-oxide-semiconductor compatible technologies, which can realize multilevel photoelectric logic computing and in situ memory simultaneously. The transistor presents stepped floating gates of perovskite quantum dots with different bandgaps and exhibits nonvolatile multilevel memory states written/erased by electrical and high-bandwidth optical signals. Meanwhile, the device can also realize logic functions such as an optoelectronic AND gate by separably programming the states of the stepped floating gates with bias and optical wavelength. A convergence of multilevel logic computing and storage is further achieved on the transistor. By demonstrating such multifunctionality in a single device, the photoelectric transistors, even with a rather large size to match photonic cells, can provide the optoelectronic microprocessors with substantially improved performances.
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Thanks to their excellent compatibility with the complementary metal-oxide-semiconductor (CMOS) process, antiferroelectric (AFE) HfO2/ZrO2-based thin films have emerged as potential candidates for high-performance on-chip energy storage capacitors of miniaturized energy-autonomous systems. However, increasing the energy storage density (ESD) of capacitors has been a great challenge. In this work, we propose the fabrication of ferroelectric (FE) Hf0.5Zr0.5O2/AFE Hf0.25Zr0.75O2 bilayer nanofilms by plasma-enhanced atomic layer deposition for high ESD capacitors with TiN electrodes. The effects of the FE/AFE thickness composition and annealing conditions are investigated, revealing that the Hf0.5Zr0.5O2 (1 nm)/Hf0.25Zr0.75O2 (9 nm) bilayer can generate the optimal ESD after optimized annealing at 450 °C for 30 min. This is mainly ascribed to the factor that the introduction of a 1 nm Hf0.5Zr0.5O2 layer enhances the formation of the tetragonal (T) phase with antiferroelectricity in the AFE Hf0.25Zr0.75O2 layer as well as the breakdown electric field of the bilayer while fixing the FE/AFE bilayer thickness at 10 nm. As a result, a ESD as high as 71.95 J cm-3 can be obtained together with an energy storage efficiency (ESE) of 57.8%. Meanwhile, with increasing the measurement temperature from 300 and 425 K, the capacitor also demonstrates excellent stabilities of ESD and ESE. In addition, superior electrical cycling endurance is also demonstrated. Further, by integrating the capacitor into deep silicon trenches, a superhigh ESD of 364.1 J cm-3 is achieved together with an ESE of 56.5%. This work provides an effective way for developing CMOS process-compatible, eco-friendly and superhigh ESD three-dimensional capacitors for on-chip energy storage applications.
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Spectrum reconstruction with filter-free microspectrometers has attracted much attention owing to their promising potential in in situ analysis systems, on-chip spectroscopy characterizations, hyperspectral imaging, etc. Further efforts in this field can be devoted to improving the performance of microspectrometers by employing high-performance photosensitive materials and optimizing the reconstruction algorithms. In this work, we demonstrate spectrum reconstruction with a set of photodetectors based on graded-band-gap perovskite quantum dot (PQD) heterojunctions using both calculation and machine learning algorithms. The photodetectors exhibit good photosensitivities with nonlinear current-voltage curves, and the devices with different PQD band gaps show various spectral responsivities with different cutoff wavelength edges covering the entire visible range. Reconstruction performances of monochromatic spectra with the set of PQD photodetectors using two different algorithms are compared, and the machine learning method achieves relatively better accuracy. Moreover, the nonlinear current-voltage variation of the photodetectors can provide increased data diversity without redundancy, thus further improving the accuracy of the reconstructed spectra for the machine learning algorithm. A spectral resolution of 10 nm and reconstruction of multipeak spectra are also demonstrated with the filter-free photodetectors. Therefore, this study provides PQD photodetectors with the corresponding optimized algorithms for emerging flexible microspectrometer systems.
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The data processing efficiency of traditional computers is suffering from the intrinsic limitation of physically separated processing and memory units. Logic-in-memory and brain-inspired neuromorphic computing are promising in-memory computing paradigms for improving the computing efficiency and avoiding high power consumption caused by extra data movement. However, memristors that can conduct digital memcomputing and neuromorphic computing simultaneously are limited by the difference in the information form between digital data and analogue data. In order to solve this problem, this paper proposes a flexible low-dimensional memristor based on boron nitride (BN), which has ultralow-power non-volatile memory characteristic, reliable digital memcomputing capabilities, and integrated ultrafast neuromorphic computing capabilities in a single in situ computing system. The logic-in-memory basis, including FALSE, material implication (IMP), and NAND, are implemented successfully. The power consumption of the proposed memristor per synaptic event (198 fJ) can be as low as biology (fJ level) and the response time (1 µs) of the neuromorphic computing is four orders of magnitude shorter than that of the human brain (10 ms), paving the way for wearable ultrahigh efficient next-generation in-memory computing architectures.
Assuntos
Computadores , Redes Neurais de Computação , Compostos de Boro , Encéfalo , Humanos , LógicaRESUMO
Thin-film transistors (TFTs) based on amorphous In-Ga-Zn-O (a-IGZO) channels present high mobility, large-area uniformity, mechanical flexibility and photosensitivity, and thus have extensive applicability in photodetectors, wearable devices, etc. However, pure a-IGZO based photosensors only exhibit a UV light response with limited sensitivity performance. By utilizing in situ interfacial hydrogen doping, it is demonstrated that the a-IGZO TFTs with the Al2O3 dielectric deposited by plasma-enhanced atomic layer deposition at room temperature (RT) have excellent photosensing performance, such as a photoresponsivity of over 6 × 105 A W-1 and a light to dark current ratio up to 107. This is attributed to spontaneous interfacial hydrogen doping into the a-IGZO channel during sputtering deposition of a-IGZO on hydrogen-rich Al2O3 films, thus generating subgap states in the band gap of IGZO. Further, color pattern imaging was achieved by employing an array of the color distinguishable devices, and flexibility was demonstrated by fabricating the TFTs onto polymer substrates. Moreover, it is also found that both the RT and 150 °C Al2O3 a-IGZO TFTs exhibit typical light-stimulated synaptic behaviors, including excitatory post-synaptic current and pair-pules facilitation, etc., and the memory time of the synaptic devices can be easily modulated by the degree of the interfacial hydrogen doping.
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Optoelectronic devices for light or spectral signal detection are desired for use in a wide range of applications, including sensing, imaging, optical communications, and in situ characterization. However, existing photodetectors indicate only light intensities, whereas multiphotosensor spectrometers require at least a chip-level assembly and can generate redundant signals for applications that do not need detailed spectral information. Inspired by human visual and psychological light perceptions, the compression of spectral information into representative intensities and colours may simplify spectrum processing at the device level. Here, we propose a concept of spectrum projection using a bandgap-gradient semiconductor cell for intensity and colour perception. Bandgap-gradient perovskites, prepared by a halide-exchanging method via dipping in a solution, are developed as the photoactive layer of the cell. The fabricated cell produces two output signals: one shows linear responses to both photon energy and flux, while the other depends on only photon flux. Thus, by combining the two signals, the single device can project the monochromatic and broadband spectra into the total photon fluxes and average photon energies (i.e., intensities and hues), which are in good agreement with those obtained from a commercial photodetector and spectrometer. Under changing illumination in real time, the prepared device can instantaneously provide intensity and hue results. In addition, the flexibility and chemical/bio-sensing of the device via colour comparison are demonstrated. Therefore, this work shows a human visual-like method of spectrum projection and colour perception based on a single device, providing a paradigm for high-efficiency spectrum-processing applications.