WO2022086449A1 - Photodétecteur à polymère ferroélectrique, points quantiques et graphène - Google Patents

Photodétecteur à polymère ferroélectrique, points quantiques et graphène Download PDF

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Publication number
WO2022086449A1
WO2022086449A1 PCT/SG2021/050638 SG2021050638W WO2022086449A1 WO 2022086449 A1 WO2022086449 A1 WO 2022086449A1 SG 2021050638 W SG2021050638 W SG 2021050638W WO 2022086449 A1 WO2022086449 A1 WO 2022086449A1
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layer
photodetector
quantum dots
graphene
ferroelectric polymer
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PCT/SG2021/050638
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English (en)
Inventor
Barbaros Oezyilmaz
Chee Tat TOH
Qian Yang
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National University Of Singapore
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L31/08—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof in which radiation controls flow of current through the device, e.g. photoresistors
    • H01L31/10—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof in which radiation controls flow of current through the device, e.g. photoresistors characterised by potential barriers, e.g. phototransistors
    • H01L31/101—Devices sensitive to infrared, visible or ultraviolet radiation
    • H01L31/102—Devices sensitive to infrared, visible or ultraviolet radiation characterised by only one potential barrier
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L31/0248—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies
    • H01L31/0352—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies characterised by their shape or by the shapes, relative sizes or disposition of the semiconductor regions
    • H01L31/035209—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies characterised by their shape or by the shapes, relative sizes or disposition of the semiconductor regions comprising a quantum structures
    • H01L31/035218—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies characterised by their shape or by the shapes, relative sizes or disposition of the semiconductor regions comprising a quantum structures the quantum structure being quantum dots
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K85/00—Organic materials used in the body or electrodes of devices covered by this subclass
    • H10K85/20—Carbon compounds, e.g. carbon nanotubes or fullerenes
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y20/00—Nanooptics, e.g. quantum optics or photonic crystals
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y30/00—Nanotechnology for materials or surface science, e.g. nanocomposites

Definitions

  • This invention relates to a photodetector comprises ferroelectric polymer, quantum dots and graphene, and a method of fabricating the same. More particularly, this invention relates to a photodetector having a photoactive structure comprises quantum dots and a ferroelectric polymer layer, formed on a graphene layer.
  • Photodetectors are sensors that can convert photon energy of light into electrical signal. They are essential elements in various applications, such as optical communication, thermal imaging, biometric system, surveillance security system, etc. Semiconductor-based photodetectors typically have a p-n junction that converts light photons into current. The absorbed photons make electron-hole pairs in the depletion region.
  • Quantum dots e.g. PbS
  • PbS Quantum dots
  • quantum dots have poor conductivity in transporting photocurrent.
  • graphene is a thin, strong and yet flexible material that has high conductivity and lower Fermi level than quantum dots. Therefore, graphene with high carrier mobility is an excellent candidate to transport the photoinduced holes from quantum dots.
  • holes from quantum dots to graphene need to transport across the interface between the quantum dots and graphene. The interface has many trap sites for holes which may cause the recombination of electrons and holes, thus hindering the efficiency of holes transport from quantum dots. As a result, photodetectors with quantum dots and graphene always found to have low efficiency.
  • the state of the art photodetectors with graphene and quantum dots will require a chemical etchant to transfer graphene from its growth substrate and then depositing quantum dots on the transferred graphene layer.
  • the graphene transferred by the chemical etching method inevitably contains contaminations/residues from the etchant and intermediate supporting polymer film. Therefore, due to the underlying problems of the chemical etching transfer method, the state of the art photodetectors are generally have poor reproducibility and uniformity issue of the graphene/quantum dots. In view of the above, a more efficient photodetector without using chemical etchant or intermediate layer is highly desired.
  • a photodetector that comprises a ferroelectric polymer layer, quantum dots and graphene, and a method of fabricating the same.
  • a ferroelectric polymer layer is utilised to define an internal electric field that extends into the graphene layer to enhance the transport of photoinduced holes from the quantum dots to the graphene layer so that more photocurrent can be generated thereby improving the photoresponse of the photodetector.
  • the photoresponse of the photodetector is improved significantly through the use of a ferroelectric polymer layer that defines an internal electric field to facilitate the transport of holes from the quantum dots to the graphene layer.
  • sensibility and reliability of the photodetector are improved as polarization of the ferroelectric polymer layer is controllable to allow for tuning of the Fermi level of the graphene towards an optimum Dirac point to enhance carrier mobility in the graphene layer.
  • the ON/OFF state of the photodetector can be easily controlled by changing the orientation of the internal electric field of the ferroelectric polymer layer.
  • the stack structure of the ferroelectric polymer, quantum dots and graphene can be transferred onto any arbitrary target substrate including semiconductor material, conductive material, polymer film, and paper.
  • a photodetector comprising: a graphene layer formed on a substrate; and a photoactive structure comprising quantum dots and a ferroelectric polymer layer, formed on the graphene layer, and configured to generate carrier holes when illuminated.
  • the ferroelectric polymer layer has an internal electric field that extends into the graphene layer to facilitate transport of photoinduced carrier holes from the photoactive structure into the graphene layer, the internal electric field being generated by a polarization of the ferroelectric polymer layer
  • the photoactive structure may have two different configurations.
  • the quantum dots of the photoactive structure are formed as a layer on the graphene layer, and the ferroelectric polymer layer of the photoactive structure is formed on the layer of the quantum dots.
  • the quantum dots of the photoactive structure are embedded within the ferroelectric polymer layer of the photoactive structure.
  • the polarization level of the ferroelectric polymer layer depends on a Fermi level of the graphene.
  • the photodetector is turned on or off based on an orientation of the internal electric field of the ferroelectric polymer layer.
  • the ferroelectric polymer layer comprises polyvinylidene fluoride (PVDF) or poly(vinylidene fluoride-co-trifluoroethylene) (PVDF-TrFE).
  • PVDF polyvinylidene fluoride
  • PVDF-TrFE poly(vinylidene fluoride-co-trifluoroethylene)
  • the ferroelectric polymer layer has a thickness between 10 nm and 100 pm.
  • the ferroelectric polymer layer embedded with the quantum dots has a thickness between 10 nm and 1 pm.
  • the quantum dots comprise lead sulphide, cadmium sulphide, lead selenide, cadmium selenide, zinc sulphide, zinc selenide, or silicon.
  • the quantum dots have diameters between 1 nm and 50 nm.
  • the graphene layer is p-doped.
  • the substrate comprises a semiconductor material, a conductive material, a polymer film, or a paper.
  • a method of fabricating a photodetector comprising the steps of: forming a graphene layer on a copper layer; forming a layer of quantum dots on the graphene layer; forming a ferroelectric polymer layer on the layer of quantum dots; laminating a thermal release tape (TRT) on the ferroelectric polymer layer; removing the copper layer, using a mechanical delamination process, to produce a stack structure comprising the graphene layer, the layer of quantum dots, the ferroelectric polymer layer, and the TRT ; transferring the stack structure onto a substrate; and removing, using hot pressing, the TRT from the stack structure.
  • TRT thermal release tape
  • the ferroelectric polymer layer has an internal electric field that extends into the graphene layer to facilitate transport of photoinduced carrier holes from the photoactive structure into the graphene layer, the internal electric field being generated by a polarization of the ferroelectric polymer layer.
  • the graphene layer is grown by chemical vapour deposition.
  • Fig. 1A is a schematic view a photodetector in accordance with a first embodiment of this invention.
  • Fig. 1 B is a schematic of a photodetector in accordance with a second embodiment of this invention.
  • Fig. 2A shows the internal electric field of the ferroelectric polymer during ON state.
  • Fig. 2B shows the internal electric field of the ferroelectric polymer during OFF state.
  • Fig. 3 shows the photoresponse comparison of the photodetector of this invention (one layer of quantum dots) with the state of the art photodetectors (one, two and three layers of quantum dots).
  • Fig. 4A shows the energy level diagram of the interface between the intrinsic graphene and quantum dots of the photodetector of this invention.
  • Fig. 4B shows the energy level diagram of the interface between the p-doped graphene and quantum dots of the photodetector of this invention.
  • Fig. 5 shows the photoresponse of the photodetector of this invention at different polarization of the ferroelectric polymer.
  • Fig. 6 shows a fabrication process of the photodetector of this invention. Description of Embodiments
  • Fig. 1 A and 1 B show photodetector 100 in accordance with a first embodiment and a second embodiment of this invention respectively.
  • Photodetector 100 comprises substrate 102 with electrical contacts, a graphene layer 104 on top of substrate 102, and a photoactive structure 106 on top of graphene layer 104.
  • Photoactive structure 106 comprises a ferroelectric polymer layer 106A and quantum dots 106B.
  • photoactive structure 106 comprises at least one layer of quantum dots 106B formed on graphene layer 104 and a ferroelectric polymer layer 106A formed on the at least one layer of quantum dots 106B.
  • photoactive structure 106 with only one layer of quantum dots 106B is shown in Fig. 1A.
  • photoactive structure 106 comprises a ferroelectric polymer layer 106A with quantum dots 106B embedded therein to form a single composite layer on graphene layer 104. Therefore, the second embodiment can achieve a thinner configuration than the first embodiment.
  • Graphene layer 104 has ultrahigh conductivity (carrier mobility) and lower Fermi level compared to quantum dots 106B.
  • Graphene layer 104 serves as a carrier channel for collecting photoinduced holes from quantum dots 106B.
  • the interface or junction between quantum dots 106B and graphene layer 104 will hinder the holes transport from quantum dots 106B to graphene layer 104.
  • ferroelectric polymer layer 106A is utilised to define an internal or built-in electric field that may extend into graphene layer 104 to facilitate the holes transfer so that more photocurrent can be generated in the graphene channel.
  • Ferroelectric polymer layer 106A is a dielectric material in which polarization may remain permanently even after removing the applied electric field. The direction of the dipole moment can also be switched by applying electric field.
  • Ferroelectric polymer layer 106A can be made of a homopolymer such as polyvinylidene fluoride (PVDF), or a copolymer such as poly(vinylidene fluoride-co-trifluoroethylene) (PVDF-TrFE), or other suitable materials.
  • PVDF polyvinylidene fluoride
  • PVDF-TrFE poly(vinylidene fluoride-co-trifluoroethylene)
  • ferroelectric polymer layer 106A may have a thickness between 10 nm to 100 pm.
  • ferroelectric polymer layer 106A embedded with quantum dots 106B may have a thickness between 10 nm to 1 pm.
  • Quantum dots 106B can be made of lead sulphide, cadmium sulphide, lead selenide, cadmium selenide, zinc sulphide, zinc selenide, silicon or other suitable materials.
  • Quantum dots layer 106B can be synthesized into different sizes with diameters between 1 nm to 50 nm.
  • Graphene layer 104 can be grown by chemical vapour deposition (CVD) and have a thickness between 0.3 nm to 2 nm.
  • Substrate 102 can be a semiconductor material, a conductive material, a polymer film (e.g. PET), a sheet of paper, or any suitable materials.
  • this invention introduces ferroelectric polymer layer 106A (e.g. PVDF or PVDF-TrFE) to solve the inefficient holes transport from quantum dots 106B to graphene layer 104 as ferroelectric polymer layer 106A can form a favourable internal or built-in electric field to facilitate the holes transfer between quantum dots 106B and graphene layer 104.
  • ferroelectric polymer layer 106A e.g. PVDF or PVDF-TrFE
  • photodetector 100 of this invention can achieve the same photoresponse with a thinner quantum dots layer, and achieve a higher photoresponse with the same thickness of quantum dots layer. Hence, this invention has a significant technical advancement.
  • this invention utilises the internal electric field in a polarized ferroelectric polymer layer 106A to enhance the holes transport.
  • the internal electric field 1 10 facilitates the holes transfer from quantum dots 106B to graphene layer 104 when the field direction is pointing from quantum dots 106B to graphene layer 104 (i.e. ON state), while prohibiting the holes transfer when the field is in the opposite direction (i.e. OFF state), as shown in Fig. 2A and 2B.
  • the stable internal electric field in ferroelectric polymer layer 106A after polarization can act as a continuous enhancing film for photodetector 100, and the ease of reorienting the polarization of ferroelectric polymer layer 106A can control the ON/OFF state of photodetector 100 easily.
  • OFF state is the initial state of photodetector 100 before illumination. This ensures no holes carriers are transported to graphene layer 104 for a very low dark current value.
  • holes transfer out of quantum dots 106B, leaving quantum dots 106B become electron rich. This in turn flips the polarization of ferroelectric polymer layer 106A, creating a strong build-in (internal) field that further depletes more holes from quantum dots 106B, as shown in Fig. 2A.
  • a voltage pulse can be applied to replenish the holes within quantum dots 106B, thereby switching the polarization of ferroelectric polymer layer 106A and resetting it to OFF state.
  • the efficiency of photodetector 100 is exemplified in the following.
  • the built-in (internal) electric field 110 in ferroelectric polymer layer 106A is pointing from quantum dots 106B to graphene layer 104 (Fig. 2A)
  • the holes gain extra energy to transport.
  • the holes will transport along the electric field direction. This reduces the charge recombination of electrons and holes before the holes can reach graphene layer 104, thus increasing the photocurrent. Therefore, more photoinduced holes can transport across the interface of quantum dots 106B and graphene 104, thereby improving photoresponse.
  • the present invention utilises ferroelectric polymer layer 106A with built-in electric field to improve the transport efficiency of photoinduced holes, without the need to increase the thickness of the quantum dot layer. Therefore, photoresponse of the present invention is much higher than the state of the art photodetectors.
  • Quantitative measurement of the photoresponse of photodetector 100 (first embodiment) is illustrated in Fig. 3.
  • Graphene resistance change with light compared to without light, AR/R(%), is used to show the photoresponse. The higher of AR/R means the better photoresponse.
  • AR/R of photodetector 100 of the present invention with one layer of quantum dots 106B (star mark) is 36.1% which is about four times higher than AR/R of the state of the art photodetector with same one layer of quantum dots (9.4%, triangle mark), and also higher than the state of the art photodetectors with two layers of quantum dots (22.4%, circle mark) and three layers of quantum dots (28.1 %, square mark).
  • This comparison shows that photodetector 100 of the present invention is much more efficient than the state of the art photodetectors.
  • This invention has optimal performance and reliable sensitivity as compared to the state of the art photodetectors.
  • Fermi level of graphene is at the Dirac point, carrier mobility in graphene is the highest, as shown in Fig. 4A.
  • quantum dots are deposited on graphene, there is a shift in the Fermi level of graphene away from the Dirac point, leading to n-doped graphene. This causes the photodetecting measurement to be carried out when the carrier mobility in graphene is decreased.
  • graphene is p-doped before depositing quantum dots, the n-doping by the quantum dots will drive Fermi level of graphene towards Dirac point, leading to the highest mobility of carriers in graphene, as shown in Fig. 4B.
  • Another reason for high sensitivity is due to p-doped graphene having available electronic states that allow for holes to transport from quantum dots 106B through graphene layer 104 to the device circuit.
  • holes are excited out of quantum dots 106B and transported into graphene layer 104.
  • holes are transported from graphene layer 104 to replenish the holes in quantum dots 106B.
  • This change in holes carriers will shift the Fermi level of graphene away and towards the charge neutrality (Dirac) point of graphene band structure.
  • Dirac charge neutrality
  • very few holes are able to transport through graphene, leading to very low photocurrent measured.
  • high carrier densities are observed for high photocurrent. This large measurable change in photocurrent is important for the uniquely high sensitivity of photodetector 100 of this invention.
  • the ON/OFF state of photodetector 100 can be controlled easily and accurately.
  • the polarization in ferroelectric polymer layer 106A is changed to the opposite direction (Fig. 2B)
  • the holes transport from quantum dots 106B to graphene layer 104 is significantly prohibited.
  • the photoinduced holes will stay in quantum dots 106B instead of transferring to graphene layer 104.
  • photodetector 100 is turned off for detecting.
  • the polarization may be controlled by having an externally applied electric field or the ferroelectric dipoles may switch in response to the charged state of quantum dots 106B.
  • Quantitative measurement of the photoresponse of photodetector 100 of this invention (second embodiment) at different polarization of ferroelectric polymer layer 106A (e.g. PVDF or PVDF-TrFE) is shown in Fig. 5.
  • ferroelectric polymer layer 106A e.g. PVDF or PVDF-TrFE
  • the AR/R(%) of photodetector 100 from fully positive polarization (24.8%, star mark) to non-polarization (12.4%, circle mark) then to fully negative polarization (4.9%, triangle mark) is changing from the highest to the lowest. This shows that polarization of ferroelectric polymer layer 106A can be used to control the photoresponse of photodetector 100.
  • Photodetector 100 of this invention is formed by a simple dry fabrication process that able to provide higher yield, lower cost, and patterning ability.
  • the use of the unique dry transfer process of graphene (coupled with quantum dots) results in no residues from the chemical etchant and/or intermediate supporting film on the device. Without using chemical etchant or intermediate layer, the process of this invention is more efficient and economical compared to the state of the art method.
  • the graphene dry transfer process can achieve large area transfer and compatible with industry grade equipment. Therefore, the graphene/quantum dots produced by the process of this invention will have higher uniform electrical properties and device performance, and more scalable-ready than the state of the art method.
  • the switchable polarization of ferroelectric polymer layer 106A in response to the quantity and charged state of quantum dots 106B, as well as the ability to minimize defects induced from graphene transfer, ensures uniform readout from all pixels in the photodetector array.
  • ferroelectric polymer layer 106A also acts as a supporting film for the CVD grown graphene.
  • the built-in electric field in ferroelectric polymer layer 106A can decrease or increase the binding energy between graphene and copper locally, due to the electrostatic doping in graphene. Therefore, by selectively polarizing ferroelectric polymer layer 106A, graphene layer 104 can be formed with a designed pattern.
  • the integration of transfer, pattern and device fabrication of this invention can be achieved in one facile process.
  • the fabrication process 600 of photodetector 100 (first embodiment) is shown in Fig. 6.
  • a graphene layer 104 is formed on copper layer 112 by chemical vapour deposition (CVD) or other suitable method.
  • a layer of quantum dots 106B e.g. PbS
  • a ferroelectric polymer layer 106A e.g. PVDF or PVDF-TrFE
  • a thermal release tape (TRT) 114 is laminated on ferroelectric polymer layer 106A.
  • copper layer 112 is removed using a mechanical delamination process, leaving a stack structure comprises graphene layer 104, quantum dots layer 106B, ferroelectric polymer layer 106A, and TRT 1 14.
  • This stack structure is then transferred onto substrate 102 in step (e).
  • TRT 1 14 is removed using hot pressing in step (f).
  • Graphene layer 104 on copper layer 1 12 may be first patterned by standard graphene fabrication processes, such as lithography and oxygen plasma etching. The patterned graphene layer 104 can then be removed in step (d) and transferred onto substrate 102 in step (e) with the required graphene design.
  • the stack layers of graphene 104, quantum dots 106B and ferroelectric polymer layer 106A can be transferred onto any substrates 102, such as a polymer film (e.g. polyethylene terephthalate) or a sheet of cheap paper. Therefore, this method enables transferring of graphene 104 with ferroelectric polymer layer 106A and quantum dots 106B onto SiO2/Si wafer (a typical semiconductor substrate), Au coated SiO2/Si wafer (a conductive substrate), PET film (a flexible and transparent substrate), and paper (cheap and disposable substrate).
  • SiO2/Si wafer a typical semiconductor substrate
  • Au coated SiO2/Si wafer a conductive substrate
  • PET film a flexible and transparent substrate
  • paper cheap and disposable substrate

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Abstract

Selon l'invention, un photodétecteur comprend une couche de graphène formée sur un substrat, et une structure photoactive formée sur la couche de graphène. La structure photoactive comprend des points quantiques et une couche de polymère ferroélectrique, et est conçue pour générer des trous porteurs lorsqu'elle est éclairée. La couche de polymère ferroélectrique présente un champ électrique interne qui s'étend dans la couche de graphène pour faciliter le transport de trous porteurs photo-induits à partir de la structure photoactive dans la couche de graphène, ce qui permet d'améliorer la photoréponse du photodétecteur.
PCT/SG2021/050638 2020-10-22 2021-10-21 Photodétecteur à polymère ferroélectrique, points quantiques et graphène WO2022086449A1 (fr)

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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN114823950A (zh) * 2022-05-10 2022-07-29 云南师范大学 一种基于碳量子点和贵金属纳米颗粒的光电探测器
CN114823950B (zh) * 2022-05-10 2024-06-07 云南师范大学 一种基于碳量子点和贵金属纳米颗粒的光电探测器

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