Two-dimensional Semiconductor Materials Research Articles

Vertical Dipole Dominates Charge Carrier Lifetime in Monolayer Janus MoSSe.

Two-dimensional semiconductor materials with vertical dipoles are promising photocatalysts as vertical dipoles not only promote the electron-hole separation but also enhance the carrier redox ability. However, the influence of vertical dipoles on carrier recombination in such materials, especially the competing relationship between vertical dipoles and band gaps, is not yet clear. Herein, first-principles calculations and nonadiabatic molecular dynamics simulations were combined to clarify the influence of band gap and vertical dipole on the carrier lifetime in Janus MoSSe monolayer. By comparing with the results of MoS2 and MoSe2 as well as exploring the carrier lifetime of MoSSe under strain regulation, it has been demonstrated that the vertical dipole, rather than the band gap, is the dominant factor affecting the carrier lifetime. Strikingly, a linear relationship between the carrier lifetime and vertical dipole is revealed. These findings have important implications for the design of high-performance photocatalysts and optoelectronic devices.

Near-Field Radiative Heat Transfer between Layered β-GeSe Slabs: First-Principles Approach.

The group-IV monochalcogenide monolayers, GeSe, are interesting and novel two-dimensional (2D) semiconductor materials due to their highly anisotropic physical properties. Monolayers of the different GeSe polymorphs have already had their physical properties and potential applications extensively investigated. However, few-layer homostructures, which can also be approximated as 2D systems in many cases, have not received the same attention. For this reason, in this work, we investigate the optical properties of a free-standing few-layer β-GeSe system and use this information to investigate their performance in the near-field radiative heat transfer (NFRHT). The required optical conductivity of the few-layer 2D material is calculated by using density functional theory (DFT), including spin-orbit coupling. The band structure is investigated for up to five layers, and the effective electron masses are calculated correspondingly. Using this information, both the intraband transitions due to the presence of free electrons introduced by doping and the interband transitions are considered. The contribution of the ionic vibrations is also included in calculating the optical properties because of its relevance to NFRHT through the resulting active optical phonons. With all these contributions included, more realistic predictions of the NFRHT between the layered 2D β-GeSe materials can be obtained. It is found that the heat transfer attainable with the layered system is similar to that of a single layer of β-GeSe we have obtained previously.

Electric field and strain tuned the electronic and optical properties of Zr2CO2/MoSe2 van der Waals heterojunction

Two-dimensional semiconductor materials have attracted significant research interest due to their exceptional properties in various applications. Among them, transition-metal dichalcogenides and MXenes have emerged as widely used materials in photoelectronic devices due to their excellent optical and electronic properties. In this study, we investigate the electronic and optical properties of MXene/MX2 heterojunctions by employing First Principles based on density functional theory calculations on Zr2CO2/MoSe2 van der Waals heterojunctions. The results of band structure, density of states and band alignment demonstrate that the Zr2CO2/MoSe2 heterojunction is a type-II band alignment with an indirect bandgap of 0.93 eV. We further explore the impact of electric fields and strains on their electronic and optical performance. The results show that carriers can be effectively separated for designing high-performance devices in photocatalysis under electric fields ranging from −0.5 to 0.5 V/Å and biaxial strains ranging from −4% to 10 %. The formation of the Zr2CO2/MoSe2 heterojunction allows for enhanced coefficient and a broader light absorption range compared to the individual Zr2CO2 and MoSe2 components. In consequence, this study contributes to a fundamental understanding of Zr2CO2/MoSe2 heterojunctions and their potential applications in photocatalysis.

Controlled growth of single-crystalline 2D p-type semiconductor α-MnSe for broadband photodetector

As a wide band-gap p-type semiconductor, α-MnSe has been expected to make up for the scarcity of two-dimensional (2D) semiconductor materials, which is crucial for the construction of multifunctional and miniaturized p-n junctions. Herein, we report the synthesis of single crystalline α-MnSe with its domain size, thickness and coverage controlled by hydrogen modulated CVD. The back-gate FET device was fabricated to study the electrical properties of α-MnSe. Moreover, the α-MnSe-based photodetector exhibits a broadband photo-response ranging from 532 nm to 980 nm with response times as low as ∼ 20 ms, comparable to most 2D materials.

A review: Comprehensive investigation on bandgap engineering under high pressure utilizing microscopic UV–Vis absorption spectroscopy

Bandgap engineering plays a vital role in material development and device optimization due to its significant impact on the photovoltaic and photoelectricity properties of materials. Nevertheless, it is still a great challenge to accurately control the bandgap of semiconductors to achieve the targeted properties of materials. Recently, pressure-induced bandgap regulation has emerged as a novel and effective tool to regulate bandgap, reveal the intrinsic band nature, and construct the in-depth structure–property relationships therein. In this review, the unique techniques of microscopic in situ steady-state UV–Vis absorption spectroscopy and high-pressure diamond anvil cell are introduced. This technique provides a powerful method to monitor the bandgap behaviors at high pressure. Then, the pressure-triggered bandgap responses are outlined based on several typical semiconductors, including metal halide perovskites, inorganic quantum dots, piezochromic molecular compounds, and two-dimensional semiconductor materials. The summarized structural effects on bandgap evolution and the general principles for bandgap engineering under high pressure are expected to provide guidance for further material design under ambient conditions. Microscopic absorption spectroscopy detection under high pressure is proven to be an ideal platform for developing functional materials and high-performance devices.

Thermal transports of 2D phosphorous carbides by machine learning molecular dynamics simulations

Carbon phosphide is a newly discovered two-dimensional semiconductor material which wrinkles and has a significant carrier mobility. Due to lack an accurate force field, the use of molecular dynamics to study its phonon-dominated thermal conductivity which lead to inaccurate results. At present, the use of machine learning to construct a high-precision force field has become the mainstream research method to solve this problem. The main work of this study is to construct a comprehensive training sets for Phosphorus-Doped Graphene (PCn) (n = 3, 5, 6) and to use the fitted potential to calculate the related thermal properties. The research found that (PC5) exhibited anisotropic behavior, with a thermal conductivity of 106.6 Wm−1K−1 in the y-direction and 63.6 Wm−1K−1 in the x-direction. In comparison, (PC6) and (PC3) showed isotropic behavior, with thermal conductivity of approximately 104 Wm−1K−1 and 76.83 Wm−1K−1, respectively. Compared to monolayer graphene, the lower thermal conductivity of PCn is mainly attributed to phonon-phonon scattering effects, which are limited by the regular wrinkled structure. Additionally, low-frequency phonon have been found to have a significant impact on the thermal performance of PCn. Furthermore, we investigated the influence of uniaxial strain on the PC6 and observed an increase in the thermal conductivity with increasing strain. This study used key computational and analytical techniques, including phonon dispersion relations, homogeneous nonequilibrium molecular dynamics method, spectral thermal conductivity analysis. These findings provide a theoretical basis for understanding the thermal transport properties of PCn and will guide its potential applications value.

Self-powered semitransparent WS2/LaVO3 vertical-heterostructure photodetectors by employing interfacial hexagonal boron nitride

Two-dimensional (2D) semiconductor and LaVO3 materials with high absorption coefficients in the visible light region are attractive structures for high-performance photodetector (PD) applications. Insulating 2D hexagonal boron nitride (h-BN) with a large band gap and excellent transmittance is a very attractive material as an interface between 2D/semiconductor heterostructures. We first introduce WS2/h-BN/LaVO3 semitransparent PD. The photo-current/dark current ratio of the device exhibits a delta-function characteristic of 4 × 105 at 0 V, meaning ‘self-powered’. The WS2/h-BN/LaVO3 PD shows up to 0.27 A W−1 responsivity (R) and 4.6 × 1010 cm Hz1/2 W−1 detectivity (D*) at 730 nm. Especially, it was confirmed that the D* performance improved by about 5 times compared to the WS2/LaVO3 device at zero bias. Additionally, it is suggested that the PD maintains 87% of its initial R for 2000 h under the atmosphere with a temperature of 25 °C and humidity of 30%. Based on the above results, we suggest that the WS2/h-BN/LaVO3 heterojunction is promising as a self-powered optoelectronic device.

Modifying the electronic and magnetic properties of the scandium nitride semiconductor monolayer via vacancies and doping.

In this work, the effects of vacancies and doping on the electronic and magnetic properties of the stable scandium nitride (ScN) monolayer are investigated using first-principles calculations. The pristine monolayer is a two-dimensional (2D) indirect-gap semiconductor material with an energy gap of 1.59(2.84) eV as calculated using the GGA-PBE (HSE06) functional. The projected density of states, charge distribution, and electron localization function assert its ionic character generated by the charge transfer from the Sc atoms to the N atoms. The monolayer is magnetized by a single Sc vacancy with a total magnetic moment of 3.00μB, while a single N vacancy causes a weaker magnetization with a total magnetic moment of 0.52μB. In both cases, the magnetism originates mainly from the atoms closest to the defect site. Significant magnetization is also reached by doping with acceptor impurities. Specifically, a total magnetic moment of 2.00μB is obtained by doping with alkali metals (Li and Na) in the Sc sublattice and with B in the N sublattice. Doping with alkaline earth metals (Be and Mg) in the Sc sublattice and with C in the N sublattice induces a value of 1.00μB. In these cases, either magnetic semiconducting or half-metallicity characteristics arise in the ScN monolayer, making it a prospective 2D spintronic material. In contrast, no magnetism is induced by doping with donor impurities (O and F atoms) in the N sublattice. An O impurity metallizes the monolayer; meanwhile, F doping leads to a large band-gap reduction of the order of 82%, widening the working regime of the monolayer in optoelectronic devices. The results presented herein may introduce efficient methods to functionalize the ScN monolayer for optoelectronic and spintronic applications.

Electronic and magnetic properties of transition-metal-doped monolayer B2S2 within GGA + U framework.

Considering the significant role of magnetism induction in two-dimensional (2D) semiconductor materials, we systematically investigate the effects of various dopants from the 3d and 4d transition metal (TM) series, including Ti, V, Mn, Fe, Co, Ni, Cu, Zn, Zr, Nb, Mo, Ru, Rh, Pd, Ag and Cd, on the electronic and magnetic properties of monolayer B2S2 through first-principles calculations. The calculated formation energies indicate that substitutional doping at the B site with various TM atoms could be achieved under S-rich growth conditions. What matters is that with the exception of systems doped with Cu, Tc, and Ag elements, which exhibit non-magnetic semiconductor properties, all other doped systems demonstrate magnetism. Specifically, the Cr-, Ni- and Pd-doped monolayers are magnetic half-metals, while the rest are magnetic semiconductors. We have also performed calculations of magnetic couplings between two TM atoms with an impurity concentration of 3.12%, revealing the prevalence of weak magnetic coupling in the majority of the magnetic systems examined. Moreover, the monolayers doped with Cr, Zr and Pd atoms exhibit ferromagnetic ground states. These findings strongly support the high potential for inducing magnetism in the B2S2 monolayer through B-site doping.

Effect of single vacancy defects on two-dimensional <i>δ</i>-InSe stability

The two-dimensional (2D) semiconductor material of InSe has received much attention due to its excellent electrical properties and moderate adjustable bandgap. The vacancy defects in the material affect not only the optical and electrical properties, but also the environmental stability. Compared with other phases in InSe materials, <i>δ</i>-InSe has superior material properties, however, the effect of environment on this material stabilityhas not been reported. In this work, we systematically investigate the stability of 2D <i>δ</i>-InSe material under oxygen environment based on density functional theory. The results are shown below. Firstly, in an oxygen environment, the perfect <i>δ</i>-InSe surface exhibits good inertness and stability, for O<sub>2</sub> molecules need to overcome an exceptionally high energy barrier of 1.827 eV from physical adsorption to chemical adsorption on its surface. Secondly, the presence of Se vacancies (V<sub>Se</sub>) promotes the oxidation reaction of <i>δ</i>-InSe, which only requires overcoming a low energy barrier of 0.044 eV. This suggests that the stability of <i>δ</i>-InSe in an oxygen environment is significantly reduced because of the presence of V<sub>Se</sub>. The O<sub>2</sub> molecules oxidized <i>δ</i>-InSe monolayer is beneficial to the dissociation and adsorption of H<sub>2</sub>O molecules. Finally, the oxidation rate of <i>δ</i>-InSe with In vacancies (V<sub>In</sub>) is slower, with the adsorption energy and charge transfer involved in the physical adsorption of O<sub>2</sub> molecules on the V<sub>In</sub> surface being similar to those on a perfect surface. The oxidation process needs to overcome a higher energy barrier of 1.234 eV. The findings of this study will provide theoretical guidance for better understanding the oxidation behavior of single vacancy defects in monolayer <i>δ</i>-InSe, and reference for experimental preparation of high-reliability 2D <i>δ</i>-InSe devices.

Strain-induced effects on the optoelectronic properties of ZrSe2/HfSe2 heterostructures.

Two-dimensional semiconductor materials have received much attention in recent years due to their wide variety of applications in the field of nano-optoelectronic devices. In this project, we applied stresses ranging from -6 to +6% to the ZrSe2/HfSe2 heterostructure and systematically investigated its electrical and optical properties. It is discovered that stress can effectively modulate the forbidden bandwidth of the ZrSe2/HfSe2 heterojunction; whereas, under compressive stress, the forbidden bandwidth of the material decreases further until the bandgap is zero, leading to the material's transformation from semiconductor to metal. The forbidden band gap of the ZrSe2/HfSe2 heterojunction increases with increasing horizontal biaxial tensile strain. We discovered that the light absorption performance of this heterostructure is significantly better than that of its similar monomolecular layer and that its light absorption intensity can reach an order of magnitude of 104. Under compressive and tensile stresses, the ZrSe2/HfSe2 heterojunctions exhibit different degrees of red or blue shift. The results indicate that constructing ZrSe2/HfSe2 heterojunctions and applying horizontal biaxial stresses to them can significantly modulate the optoelectronic properties of the materials. ZrSe2/HfSe2 heterojunction is a new type of high-performance photogenerated carrier transport device with a wide range of applications. The calculations in this study are carried out the first principles approach of density functional theory, as implemented in the CASTEP module of Materials-Studio2019. The researchers used an ultrasoft reaction potential to calculate the interactions between the ion core and the electrons and applied the Perdew-Burke-Ernzerhof (PBE) and the generalized gradient approximation (GGA) to perform the calculations. The Monkhorst-Pack technique was employed to create the k-point samples utilized for integration on the Brillouin zone, and the k-point grid was uniformly 6 × 6 × 1. In addition, in order to avoid interactions between the atomic layers affecting the properties and stability of the material, such interactions were prevented by adding a 30 Å vacuum layer. Using a plane-wave energy cutoff of 500 eV and the convergence accuracy of the iterative process was set to 1 × 10-5 eV to ensure the accuracy of the computational results, and in addition. The maximum stress in the lattice was limited to less than 0.05 GPa or the interaction force between neighboring atoms was lower than 0.03 eV/Å. For the calculation of the properties of the optical properties, a k-point grid of 18 × 18 × 1 is used for optimization, and the polarization direction of the material is not taken into account, considering that the material is isotropic. This study proposes to apply the Tkatchenko-Scheffler (TS) dispersion correction method in DFT-D to appropriately represent the interlayer van der Waals interaction forces to solve inaccuracies in the computation of van der Waals interactions via density functional theory.

Kretschmann-based plasmonic excitation of 2D organic semiconductor at visible wavelengths

We studied the Kretschmann-based surface plasmon resonance (K-SPR) of two-dimensional organic semiconductor materials, namely manganese (III) phthalocyanine chloride (MnPcCl) and vanadyl-2,9,16,23-tetraphenoxy-29H,31H-phthalocyanine (VOPcPhO). The K-SPR measurements indicate that VOPcPhO exhibits superior performance compared to MnPcCl, as evidenced by the stronger absorption and narrower SPR peaks. Oxygen-vanadium coupling in the central metal atom facilitates high absorption, potentially enabling strong plasmon-exciton coupling, which can be harnessed for efficient photovoltaic and optical memory devices.

Space-Confined Synthesis of Monolayer Graphdiyne in MXene Interlayer.

Graphdiyne (GDY) is an artificial carbon allotrope that is conceptually similar to graphene but composed of sp- and sp2 -hybridized carbon atoms. Monolayer GDY (ML-GDY) is predicted to be an ideal 2D semiconductor material with a wide range of applications. However, its synthesis has posed a significant challenge, leading to difficulties in experimentally validating theoretical properties. Here, it is reported that in situ acetylenic homocoupling of hexaethynylbenzene within the sub-nanometer interlayer space of MXene can effectively prevent out-of-plane growth or vertical stacking of the material, resulting in ML-GDY with in-plane periodicity. The subsequent exfoliation process successfully yields free-standing GDY monolayers with micrometer-scale lateral dimensions. The fabrication of field-effect transistor on free-standing ML-GDY makes the first measurement of its electronic properties possible. The measured electrical conductivity (5.1 × 103 S m-1 ) and carrier mobility (231.4 cm2 V-1 s-1 ) at room temperature are remarkably higher than those of the previously reported multilayer GDY materials. The space-confined synthesis using layered crystals as templates provides a new strategy for preparing 2D materials with precisely controlled layer numbers and long-range structural order.

Strain effects on the lattice thermal conductivity of monolayer CrOCl: A first-principles study

Monolayer CrOCl is an intrinsically ferromagnetic two-dimensional semiconductor material with potential applications in nano-spintronic devices, which call for fundamental studies of phonon transport. Here, we investigate the lattice thermal conductivity of monolayer CrOCl under uniaxial strain using first-principles calculations to solve the phonon Boltzmann transport equation. At 300 K, the lattice thermal conductivities of monolayer CrOCl are 47.00 Wm−1K−1 (x direction) and 123.97 Wm−1K−1 (y direction), exhibiting significant anisotropy. Applying uniaxial strains of − 2–2% to monolayer CrOCl in the x and y axes, we discovered that both compressive and tensile strains reduced the thermal conductivity of monolayer CrOCl. By analyzing the responses of heat capacity, phonon group velocity, and phonon lifetime to strain, we determined that the rapid decrease in phonon lifetime under strain is the primary cause of the decrease in thermal conductivity.

Progress in the preparation of high-quality wafer-scale monolayer and multilayer MS2 (M = Mo; W) films by CVD

MS2 (M = Mo; W), with natural atomic thickness, are typical two-dimensional (2D) semiconductor materials, which have excellent electronic/optoelectronic properties and mechanical flexible properties. With the development of semiconductor device miniaturization, much attention has been brought to MS2, especially in large-scale integrated circuits, ultra-sensitive photodetectors, and flexible electronic devices. Here, we present the recent research progress on the controllable synthesis of high-quality, wafer-scale, uniform monolayer and multilayer MS2 films by chemical vapor deposition methods, focusing on the most concerning grain orientation control and defect modulation in whole wafer, besides the pursuit of more larger wafer size in MS2 films’ preparation. We also discuss some critical issues in the process of MS2 films growth and give a brief outlook in the controllable preparation of high-quality MS2 films for device application later on.

Controllable growth of wafer-scale two-dimensional WS2 with outstanding optoelectronic properties

As one of two-dimensional (2D) semiconductor materials, transition metal dichalcogenides (TMDs) have sparked enormous potential in next-generation electronics due to their unique and excellent physical, electronic and optical properties. Controllable growth of wafer-scale 2D TMDs is essential to realize the various high-end applications of TMDs, while it remains challenging. Herein, 2 inch 2D WS2 films were successfully synthesized by ambient pressure chemical vapor deposition based on substrate engineering and space-confined strategies. WS2 nucleation density can be effectively modulated depending on the annealing conditions of sapphire substrate. The thickness of WS2 films can be controllably fabricated by adjusting the space-confined height. Moreover, our strategies are demonstrated to be universal for the growth of other 2D TMD semiconductors. WS2-based photodetectors with different thicknesses were systematically investigated. Monolayer WS2 photodetector displays large responsivity of 0.355 A W−1 and high specific detectivity of 1.48 × 1011 Jones. Multilayer WS2 device exhibits negative self-powered photoresponse. Our work provides a new route for the synthesis of wafer-scale 2D TMD materials, paving the way for high performance integrated optoelectronic devices.

Preparation and Performance Study of Photoconductive Detector Based on Bi2O2Se Film

Bi2O2Se, as a novel two-dimensional semiconductor material, has been prepared and used in the field of photodetection. Herein, Bi2O2Se nanosheets were prepared using a hydrothermal method. Bi2O2Se films were also prepared using a drop-coating method. A photoconductive detector based on the Bi2O2Se film was constructed. The influence of nanosheet size was considered. Ultrasonic crashing treatments and different drying processes were used for the improvement of device performance. The obtained results demonstrate that the Bi2O2Se film based on treated nanosheets is denser and more continuous, leading to a higher photocurrent (1.4 nA). Drying in a vacuum can further increase the photocurrent of the device (3.0 nA). The photocurrent would increase with the increase in drying temperatures, while the dark current increases synchronously, leading to a decrease in the on/off ratio. The device based on Bi2O2Se film was dried in a vacuum at 180 °C and exhibited high responsivity (28 mA/W) and detectivity (~4 × 109 Jones) under 780 nm light illumination. Together, these results provide a data foundation and vision for the further development of photodetectors based on Bi2O2Se material.

Prediction of two-dimensional materials: TeXO6 (X = transition metals):structure and electronic properties

Due to the extensive application of two-dimensional (2D) semiconductor materials in spintronics and tunable nano-mechanical devices, many researchers have invested in the research of 2D semiconductor materials, and they have obtained many excellent research results. Utilizing the first-principles calculations and Green’s function, we forecast the monolayer TeXO6 (X = Cr, Fe, Zn) as new 2D materials with various advantageous functional features. The calculation results for TeCrO6, TeFeO6, and TeZnO6 show good stability and promise prospective application potential if the materials are experimental synthesis. With applied strain, TeCrO6 possesses an indirect band gap of 1.096 eV, which is predicted to be strongly manipulabe in this work. We use the density functional theory to investigate the structure and electrical characteristics of the monolayer (X = transition metals). Detailed simulations of their energetics, atomic structures, and electronic structures under the impact of a biaxial strain have been performed. It is discovered that whereas TeCrO6 does not, TeXO6 (with X = Sc, Ti, V, Mn, Fe, Co, Ni, Cu, and Zn) exhibit spin splitting at the ground state. With the application of compressive strain, the electronic band gap narrows. These materials’ band topologies have been discovered to be more susceptible to biaxial stresses. If a strain of 8% is applied, TeFeO6 may change from semimetal to semiconductor. Under baxial strain, TeCrO6 exhibits interesting Van Hove singularities and Mexican-hat-like bands. Due to all these desirable characteristics, 2D TeXO6 is a prospective option for use in a number of technologies, particularly for spintronic and electrical devices.

Electronic band structures and optical properties of 2D XOF (X = Ga or In) oxyfluoride monolayers using density functional theory and GW approximation

The class of two-dimensional oxyfluoride monolayers is currently considered one of the most attractive nanomaterials for enhancing design and pushing the limits of different cutting-edge technologies. Two-dimensional semiconductor materials are the most promising systems for various applications in optoelectronic devices because they have a unique optical properties. We continue in this way by investigating the GW band structures and optical properties of unique 2D XOF (X = Ga or In) oxyfluoride monolayers, involving absorption, conductivity, refractive index, and dielectric function. We find no imaginary frequencies in the computed phonon spectra, indicating that these systems are dynamically stable. Furthermore, GaOF and InOF stay stable for temperatures T ≤ 840 K. The band gap of GaOF obtained with the single shot (G0W0) is larger than the band gap energy Eg of InOF. Where the direct band gap energies of GaOF and InOF are 6.1 eV and 4.8 eV, respectively. Our GW(PBE) numerical simulations demonstrate that the GaOF monolayer moves transparent once the frequency of the incoming light exceeds the plasma frequency (35.00 eV). Furthermore, InOF switches transparently once the incident light frequency exceeds the plasma frequency ∼ 35.00 eV. Interestingly, we obtain that these 2D sheets have a strong absorption coefficient in the range of ∼ 3.00–60.00 eV. They are emerging as a potential for the building blocks of the nano-size and ultra-thin optoelectronics of the future since they productively emit and absorb light.

Simulation Photosynthesis Improves the Photoresponse Performance of Cr2Ge2Te6 Nanosheets for High-Performance Self-Powered Photoelectrochemical Photodetectors

Two-dimensional (2D) semiconductor materials have been extensively studied as excellent candidates for future optoelectronic devices. Cr2Ge2Te6, as a two-dimensional semiconductor material, has attracted extensive interest in the field of photodetectors due to its excellent light absorption properties and suitable band gap. Inspired by biological photosynthesis, this study constructed a high-performance biomimetic self-powered photoelectrochemical-type flexible photodetector using liquid-stripped Cr2Ge2Te6 nanosheets as the photoanode. The device exhibits obvious self-powered photoresponse behavior and excellent photoresponse performance with a responsivity of 54.4 μA/W. Furthermore, the addition of nicotinamide adenine dinucleotide phosphate (NADPH) effectively consumes the photo-excited holes on the Cr2Ge2Te6 nanosheets to inhibit the recombination of photogenerated electron–hole pairs, and the cyclic regeneration of NADPH is realized by adding adenosine triphosphate. In addition, the flexible photodetector also exhibits excellent stability and durability, and it still maintains good photoresponse characteristics after 1000 times of bending and folding. Our work fully confirms that it is an effective means to improve the photoresponse performance of 2D materials by simulating biological photosynthesis, and it also provides theoretical and experimental guidance for the research and development of high-performance biomimetic devices.