The disclosure relates generally to semiconductor quantum dots and nanocrystals.
Semiconductor quantum dots (QDs) have potential applications in the field of integrated quantum optics including quantum-computing, quantum key distribution and secure data transmission. To date, QDs have been extensively studied for applications in single photon source, two-photon interference, and polarization entanglement. Epitaxial QDs have been proven to be promising quantum light emitters due to their scalability and integrability. The achievement of semiconductor QDs can be based on either advanced lithography, epitaxial techniques, or solution processing. Since a top-down process potentially introduces sidewall damages which lead to nonradiative recombination process, a bottom-up epitaxy process is more preferable for fabricating QDs. To date, several strategies have been utilized to grow QDs, including droplet epitaxy, Stranski-Krastanov (SK), or related processes, among which the SK growth mode has been commonly used for the synthesis of III-V semiconductor QD heterostructures.
For the extensively studied InAs/GaAs system, which has about a 7% lattice mismatch, SK growth manifests itself as an initial layer-by-layer growth with the formation of a two-dimensional (2D) wetting layer, followed by the formation of 3D dot-like structure above the InAs wetting layer. This approach, however, has several fundamental limitations. First, the presence of the wetting layer significantly reduces charge carrier confinement and introduces undesirable properties, including the hot carrier effect and reduced luminescence efficiency. Second, the optical properties of QDs have been shown to be greatly affected by the dislocation density within the substrate. For example, InGaAs quantum wells (QWs) grown on GaAs/Si with threading dislocation density of about 106-108 cm−2 show about 10 times reduction in luminescence intensity compared to QWs grown on bulk GaAs. The issue further deteriorates with III-nitride systems due to a lack of intrinsic substrates while foreign substrates typically show a large lattice mismatch and thermal expansion coefficient mismatch with the grown layers. The threading dislocation density of AlN grown on c-plane sapphire can be as high as 1011 cm−2, which is comparable to the reported density of GaN QDs spontaneously assembled on an AlN substrate.
In accordance with one aspect of the disclosure, a device includes a substrate and a heterostructure supported by the substrate, the heterostructure including a set of quantum dot structures, each quantum dot structure of the set of quantum dot structures including a semiconductor material, and a layered material disposed between the set of quantum dot structures and the substrate. The layered material includes a plurality of monolayers such that adjacent monolayers of the plurality of monolayers are bonded to one another via van der Waals forces, and the semiconductor material of each quantum dot structure of the set of quantum dot structures exhibits bonding with the layered material via van der Waals forces.
In accordance with another aspect of the disclosure, a method of fabricating a quantum dot device includes forming a layered material, the layered material including a plurality of monolayers supported by a substrate, with adjacent monolayers of the plurality of monolayers being bonded to one another via van der Waals forces, and growing epitaxially a set of quantum dot structures, each quantum dot structure of the set of quantum dot structures including a semiconductor material. Growing the set of quantum dot structures is implemented after forming the layered material such that the layered material is disposed between the set of quantum dot structures and the substrate, and the semiconductor material of each quantum dot structure of the set of quantum dot structures exhibits bonding with the layered material via van der Waals forces.
In accordance with still another aspect of the disclosure, a device includes a substrate and a heterostructure supported by the substrate, the heterostructure including a set of nanocrystals, each nanocrystal of the set of nanocrystals including a semiconductor material, and a layered material disposed between the set of nanocrystals and the substrate. The layered material includes a plurality of monolayers such that adjacent monolayers of the plurality of monolayers are bonded to one another via van der Waals forces, and the semiconductor material of each nanocrystal of the set of nanocrystals exhibits bonding with the layered material via van der Waals forces.
In accordance with yet aspect of the disclosure, a method of fabricating a device includes forming a layered material, the layered material including a plurality of monolayers supported by a substrate, with adjacent monolayers of the plurality of monolayers being bonded to one another via van der Waals forces, and growing epitaxially a set of nanocrystals, each nanocrystal of the set of nanocrystals including a semiconductor material. Growing the set of nanocrystals is implemented after forming the layered material such that the layered material is disposed between the set of nanocrystals and the substrate, and the semiconductor material of each nanocrystal of the set of nanocrystals exhibits bonding with the layered material via van der Waals forces.
In accordance with still another aspect of the disclosure, a device includes a substrate and a set of quantum dot structures supported by the substrate. Each quantum dot structure of the set of quantum dot structures includes a semiconductor material. The semiconductor material of each quantum dot structure of the set of quantum dot structures exhibits bonding with the substrate via van der Waals forces.
In connection with any one of the aforementioned aspects, the devices and/or methods described herein may alternatively or additionally include or involve any combination of one or more of the following aspects or features. The substrate includes a covalently bonded material. The layered material has a number of monolayers sufficient to screen the set of quantum dot structures from a potential field of the covalently bonded material. The heterostructure lacks a wetting layer. Each quantum dot structure of the set of quantum dot structures is bonded to one of the plurality of monolayers via van der Waals forces. The quantum dot structures exhibit multiple crystallographic orientations. The heterostructure is in contact with the substrate. Each quantum dot structure of the set of quantum dot structures is in contact with a first monolayer of the plurality of monolayers. A second monolayer of the plurality of monolayers is in contact with the substrate. The semiconductor material is a III-V material. The semiconductor material is a III-nitride material. The semiconductor material is GaN. The layered material is hexagonal boron nitride. The substrate includes polycrystalline nickel. The substrate and the layered material have a chemical composition in common. The semiconductor material includes a III-nitride material, and growing the set of quantum dot structures is implemented in a nitrogen-rich environment. Growing the set of quantum dot structures is implemented at a temperature falling in a range from about 600° C. to about 850° C. degrees Celsius. Forming the layered material includes epitaxially growing the layered material. Epitaxially growing the layered material includes implementing a growth procedure configured for van der Waals epitaxy. The substrate includes a covalently bonded material, and epitaxially growing the layered material includes implementing a growth procedure configured to grow a number of monolayers sufficient to screen the set of quantum dot structures from a potential field of the covalently bonded material. The set of quantum dot structures are not grown upon a wetting layer. The set of quantum dot structures are in contact with the substrate. The substrate includes silicon. The substrate is transparent.
For a more complete understanding of the disclosure, reference should be made to the following detailed description and accompanying drawing figures, in which like reference numerals identify like elements in the figures.
The embodiments of the disclosed devices and methods may assume various forms. Specific embodiments are illustrated in the drawing and hereafter described with the understanding that the disclosure is intended to be illustrative. The disclosure is not intended to limit the invention to the specific embodiments described and illustrated herein.
Devices having a set of semiconductor quantum dots or nanocrystals are described. The disclosed devices include a heterostructure having a layered material disposed between quantum dot structures (or nanocrystals) and a substrate. The layered material includes a plurality of monolayers bonded to one another via van der Waals forces. As a result, the semiconductor material of each quantum dot (or nanocrystal) also exhibits bonding with the layered material via van der Waals forces. In some cases, the disclosed devices and methods include or involve van der Waals quantum dots (or nanocrystals) grown on multiple monolayers of hexagonal boron nitride (hBN). Methods of fabricating such quantum dot and other devices via epitaxial growth procedures are also described.
The layered material may have a number of monolayers sufficient to screen the quantum dot structures (or nanocrystals) from a potential field of the substrate. For instance, the substrate may be composed of a covalently bonded material. During epitaxial growth of the quantum dot structures (or nanocrystals), the semiconductor material of the quantum dots (or nanocrystals) is shielded from the potential field from the covalent bonds by the monolayers. As a result, the epitaxial growth of the quantum dots (or nanocrystals) is governed by van der Waals interactions. Covalent epitaxial growth is thus avoided.
The issues noted above can be addressed in van der Waals (vdW) based heterostructures, in which the atomic interactions between the grown materials and substrates are significantly weakened. This weak interaction has enabled the successful exfoliation of III-V optoelectronic materials epitaxially integrated on substrates coated by 2D materials such as graphene and hBN, which has shown promising applications for next-generation flexible and wearable devices. Moreover, it has been shown that the potential field from covalent-bonded substrates can be screened by a monolayer of graphene although that from ionic-bonded substrates can penetrate through a few layers of graphene. Such field penetration can be substantially attenuated by two-dimensional (2D) hexagonal boron nitride (hBN), a compound semiconductor with a hexagonal type crystalline structure and strong, in-plane, sp2 ionic bonding. hBN has been shown to be the best insulating material to enhance the mobility of graphene and can significantly suppress the carrier inhomogeneities in transition metal dichalcogenides.
As described herein, vdW based heterostructures are used to support the synthesis of vdW bonded QDs and nanocrystals.
Described herein are examples of complete vdW epitaxy of GaN. Such epitaxy is achieved when the thickness of hBN on polycrystalline nickel is equal to, or above, two monolayers. Such epitaxy may be implemented under nitrogen-rich growth conditions instead of the conventional metal-rich growth conditions. The examples establish the successful demonstration of epitaxy and morphology control of wetting layer free GaN QDs on layered hBN. Detailed structural characterizations show that GaN QDs are free of threading dislocations and stacking faults. Unlike QDs covalently bonded to substrates, multiple crystallographic orientations were observed in QDs bonded with hBN through vdW interactions. Highly efficient radiative recombination process was measured from GaN QDs on hBN with the photoluminescence (PL) emission intensity 4 times stronger compared with QDs synthesized on AlN and Si substrates while the QD density on hBN is nearly two orders of magnitude lower, confirming the extremely high quality of van der Waals GaN QDs grown on a plurality of monolayers of hBN (e.g., few layer hBN).
Although described in connection with light emitting and/or optoelectronic devices, the disclosed methods and devices may be applied to a wide variety of electronic and other devices. For instance, the disclosed devices may be configured for quantum computing and other electronic functions and applications.
Although described in connection with examples having GaN quantum dot structures, the disclosed devices and methods may include or involve quantum dot structures of varying composition. For instance, the disclosed methods and devices may include or involve other III-nitride materials, other III-V materials, or other semiconductor materials. In some cases, the quantum dot structures are composed of, or otherwise include, III-nitride semiconductor materials, such as InN and AlN, as well as their alloys.
The compositions of other elements or components of the disclosed devices may also vary. For instance, the disclosed devices are not limited to a particular substrate material or a particular type of layered material disposed between the substrate and the quantum dot structures. While the disclosed devices and methods are described in connection with nickel substrates, other substrate materials may be used, including, for instance, graphene and graphite. While the disclosed devices and methods are described in connection with hBN monolayers, other layered materials may be used, including, for instance, Molybdenum disulfide (MoS2), Molybdenum diselenide (MoSe2), Tungsten disulfide (WS2), Tungsten diselenide (WSe2), and graphene.
The substrate of the disclosed devices may or may not correspond with the growth substrate, or the substrate on which the heterostructures of the disclosed devices are grown. For instance, the heterostructures may be transferred to another substrate, such as a GaN, Si, or sapphire substrate, after growth of the heterostructures.
The substrate may or may not have a composition in common with the layered material of the heterostructure. For instance, the substrate may be composed of, or otherwise include, graphene, silicon, sapphire, nickel, or copper, while the layered material may be composed of, or otherwise include, hexagonal BN (hBN), graphene, MoS2, WS2, or WSe2.
The configuration, construction, fabrication, and other characteristics of the heterostructures may also vary from the examples described. For instance, the heterostructures may include any number of epitaxially grown layers.
Although described in connection with MBE growth procedures, additional or alternative non-sputtered epitaxial growth procedures may be used. For instance, metal-organic chemical vapor deposition (MOCVD) and hydride vapor phase epitaxy (HVPE) growth procedures may be used. Still other procedures may be used, including, for instance, pulsed laser deposition procedures.
In the examples described below, multiple monolayers of two-dimensional (2D), layered hBN were epitaxially grown on polycrystalline nickel in a Veeco GENxplor MBE system equipped with a radio frequency nitrogen plasma source and an e-beam source. Further details regarding the growth procedures of the hBN monolayers are provided below. The resulting hBN monolayers were configured as flakes, which feature triangular domains with dimensions of about 10 μm on the polycrystalline nickel. The number of layers is identifiable based upon the contrast in the imaged area. In these examples, the center of the hBN triangle was thicker than the edges. The as-grown samples were then transferred to a Veeco GEN II system for subsequent GaN epilayer/QD growth.
Part (d) of
Further details regarding the subject matter of
To identify the thickness of the hBN layered material that is capable of completely screening the potential field of the underlying polycrystalline nickel, the epitaxy of a GaN film was first attempted under conventional metal rich growth conditions. Detailed growth parameters are provided below. Based on the morphology differences across the as-grown materials, regions with and without hBN can be readily distinguished. As shown in
Previous studies have shown that initial nucleation of GaN on hBN is almost impossible due to the sp2 orbital hybridization of hBN and its absence of dangling bonds unless intentionally introducing defects through surface treatment such as plasma treatment. Therefore, the lack of nucleation establishes that the hBN is of pristine quality and low defect density. The nucleation and formation between the magenta and green dashed lines are likely due to the potential field of Ni substrate penetrating a single monolayer of hBN. Meanwhile, in regions where the hBN thickness is equal to or greater than two monolayers, the growth becomes complete vdW epitaxy, in which adatom nucleation, i.e., growth of GaN on hBN becomes extremely difficult under the conventional metal rich conditions, as shown in
Epitaxy of GaN QDs on the hBN layered material was performed under nitrogen rich conditions and elevated temperatures. In some case, the growth temperature falls in a range from about 600° C. to about 850° C., but other temperatures may be used in connection with, for instance, other semiconductor materials. Epitaxial growth of GaN QDs using similar conditions but on AlN and Si substrates was also performed for purposes of comparison.
electron beam was aligned along the [1
Crystallographic orientation between the GaN QDs and the hBN monolayers were characterized by detailed STEM imaging and fast Fourier transform (FFT) analysis. As shown in
Morphology control of the GaN QDs on the hBN monolayers was investigated by varying the growth durations and III/N ratios with the corresponding dot density, mean aspect ratio and thickness, as summarized in Table I.
)
1.6 × 1010
indicates data missing or illegible when filed
The crystallographic orientations between the GaN QDs and hBN monolayers were further investigated by increasing growth duration to 50 mins, at which the GaN QDs evolves into faceted-nanocrystals due to anisotropies in the surface energies in the different directions. As shown in the top-view SEM image of
Based on these results, analysis on the crystallographic alignment between GaN QDs and hBN is provided. The in-plane lattice constant is 0.25 nm for hBN and 0.3189 nm for GaN. The out-of-plane lattice constant is 0.5189 nm for GaN. For horizontal nanocrystals, along the <11
The optical properties of the GaN QDs on hBN and AlN materials or substrates were then investigated through detailed PL measurements, in which a pulsed ArF excimer laser with excitation photon energy of 6.42 eV was utilized.
Temperature dependent measurements were performed on the QDs of samples A and B. As shown in
To further confirm this, power-dependent PL measurements were performed at room temperature. The excitation power was varied over 2-3 orders of magnitude. The following set of rate equations was utilized to analyze the experimental data and the radiative and nonradiative recombination processes:
in which G is the steady state generation/recombination rate, IPL is the integrated PL intensity, n is the photogenerated carrier concentration within hBN, and θ is a constant determined by the measurement setup. A is the nonradiative recombination coefficient, B is the radiative recombination coefficient and C is the coefficient related to Auger recombination, and IPL is the integrated PL intensity. Here G can be further expressed as:
in which Pex, Aspot and Eph are the laser excitation power, excitation area, and excitation photon energy, respectively. α and R are the absorption coefficient and Fresnel reflection coefficient of bulk GaN and the substrate, respectively. In this study, we used α=2.6×105 cm−1 based on previous reports, R=0.3 for hBN on nickel and R=0.4 for AlN on sapphire determined by reflection measurements. Based on equation (2), one could express n as a function of IPL0.5. Then, θ can be determined with equations (2) and (3), assuming the IQE at 13 K to be unity. Then, the relation between G and IPL can be studied with A/B0.5 and C/B1.5 as fitting parameters which vary only with temperature.
The examples described herein show that 2D, layered hBN is a useful supporting material or substrate for GaN QD growth. The vdW epitaxy of GaN QDs on the layered hBN has been achieved under nitrogen rich growth conditions. Wetting layer free GaN QDs with controllable size and density have been successfully grown on hBN. Unique structural and optical properties were observed from GaN QD/hBN heterostructures. Unlike the fixed crystallographic alignment in QDs covalently bonded to substrates, multiple orientations were observed from QDs on hBN, in which the [0001] direction of wurtzite GaN is parallel to either the <1120> or [0001] directions of the hBN flakes. The two materials are strained to accommodate a 2% misfit ensuring a certain lattice coincidence. Moreover, PL intensity obtained from GaN QDs/hBN is 4 times stronger than that of QDs grown on AlN and Si substrates despite the significantly reduced QD density, showing a highly efficient radiative recombination process. Temperature and power-dependent measurements also show that QDs on hBN are free of localized states and have significantly less Shockley-Reed-Hall recombination. These results provide unambiguous evidence that the use of hBN substrate can significantly improve the optical quality of QDs and provide a new strategy for next-generation high-performance quantum light sources.
The method 600 may begin with an act 602 in which a substrate is prepared and/or otherwise provided. In some cases, the act 602 includes providing a nickel substrate (e.g., a polycrystalline nickel substrate) in an act 604. Alternative or additional materials may be used, including, for instance, graphene or graphite. Still other materials may be used, including, for instance, BN.
The substrate may be cleaned in an act 606. For instance, the substrate may be cleaned via dips in acetone, methanol, and DI water. Organic impurities may thus be removed. In some cases, a native or other oxide layer may be removed from a substrate surface in an act 608. Additional or alternative processing may be implemented in other cases, including, for instance, degassing (e.g., via thermal degassing), doping or deposition procedures. The substrate thus may or may not have a uniform composition. The substrate may be a uniform or composite structure.
In an act 610, a layered material is formed. The layered material includes a plurality of monolayers, as described herein. As a layered material, adjacent monolayers of the plurality of monolayers being bonded to one another via van der Waals forces. In some cases, the monolayers are epitaxially grown in a growth chamber. The monolayers are thus formed on, or otherwise supported by, the substrate. In some cases, one of the monolayers is in contact with the substrate. In other cases, an intermediary layer is disposed between the semiconductor layer and the substrate. The intermediary layer may be composed of, or otherwise include, graphene, MoS2, or other layered materials.
As described herein, the layered material may have a thickness sufficient to support the van der Waals epitaxy of the quantum dot structures of the heterostructure. For instance, in cases in which the substrate is composed of, or otherwise includes, a covalently bonded material, the act 610 may include implementing a growth procedure configured to grow a number of monolayers sufficient to screen the set of quantum dot structures from a potential field of the covalently bonded material.
Epitaxially growing the layered material may include implementing a growth procedure configured for van der Waals epitaxy. For instance, the growth procedure may be configured for growth of hBN monolayers in an act 612. In some cases, the act 610 includes implementation of a plasma-assisted MBE procedure in an act 614. For instance, the layers grown in the act 614 (and/or other growth acts described herein) may use a Veeco GENxplor MBE system, equipped with a radio frequency (RF) nitrogen plasma source for active nitrogen supply (N′). Alternative or additional procedures may be implemented, including, for instance, a MOCVD procedure in an act 616.
The layered material may be composed of, or otherwise include, hBN. Alternative or additional layered materials may be formed in the act 610. For instance, monolayers of MoS2 and MoSe2 may be formed. Still other layered materials may be formed, including, for instance, graphene, MoSe2, WS2, or WSe2. The layered material and the substrate may or may not have a chemical composition in common.
Further details regarding examples of the epitaxial growth or other formation of the layered material are set forth in Laleyan et al., “Effect of growth temperature on the structural and optical properties of few-layer hexagonal boron nitride by molecular beam epitaxy,” Vol. 26, No. 18|3, Optics Express, pp. 23031-23039 (2018), the entire disclosure of which is hereby incorporated by reference.
The method 600 includes an act 618 in which a set of quantum dot structures or nanocrystals of the heterostructure are epitaxially grown. Each quantum dot structure (or nanocrystal) is composed of, or otherwise includes, a semiconductor material. In some cases, the quantum dot structures (or nanocrystals) grown in the act 618 are composed of, or otherwise includes, a III-nitride semiconductor material, such as GaN, but alternative or additional semiconductor materials may be used, including, for instance, other III-nitride semiconductor materials, such as InN and AlN and alloys thereof. Still other III-V materials and other semiconductor materials may be used.
Growing the set of quantum dot structures (or nanocrystals) is implemented after forming the layered material in the act 610 such that the layered material is disposed between the set of quantum dot structures and the substrate and, as described herein, such that the semiconductor material of each quantum dot structure of the set of quantum dot structures exhibits bonding with the layered material via van der Waals forces. The set of quantum dot structures are thus not grown upon a wetting layer, as also described herein.
The act 618 may include an act 620 in which the semiconductor layer is grown via implementation of an MBE procedure. Alternatively, a MOCVD procedure is implemented in an act 622. In either case, the growth may be continued in the same chamber used in the act 610 is used to grow the layered material.
In some cases, the act 618 includes an act 624 in which the epitaxial growth is implemented in a nitrogen-rich environment, e.g., under nitrogen-rich conditions. In one example, the radio-frequency nitrogen plasma source was employed at a power 350 W and with a Nitrogen flow rate in the range of 0.8-1 sccm. The beam equivalent pressure (BEP) of Ga is about 3 e-8 Torr. The nitrogen and Ga shutters were opened simultaneously without any seeding processes. In that example, GaN QDs were grown for 20 minutes at a thermal couple reading of 845° C. on a 1 cm-by-1 cm hBN/Ni substrate.
Other growth temperatures may be used. For instance, growing the set of quantum dot structures may be implemented at a temperature falling in a range from about 600° C. to about 850° C. degrees Celsius, but other growth temperatures may be used (e.g., in connection with the growth of other semiconductor materials). Other growth parameters may vary as well.
The method 600 may include an act 626 in which the heterostructure or a portion thereof (e.g., the quantum dot structures) is transferred from a growth substrate to another substrate (e.g., a device substrate). The device substrate may have a composition and/or other characteristics unsuitable (or less suitable) for growth of the heterostructure, but well-suited (or more well-suited) for operation or application. For instance, the device substrate may be flexible or bendable or have other structural characteristics tailored for a device application. Alternatively or additionally, the device substrate may have one or more optical or other electromagnetic characteristics tailored for a device application, such as being transparent (or opaque) or conducting (or non-conducting). As used herein, terms such as “transparent” and “conducting” are used in the context of the device functionality or application such that, for instance, the device substrate is transparent at wavelengths relevant to the functionality or application of the device. Transfer to a device substrate may be useful for additional or alternative purposes, including, for instance, hetero-integration, e.g., with one or more other structures, layers, or other elements. For example, the quantum dot structures may be transferred to a device substrate to function as active materials or components. Alternatively, the quantum dot structures may be transferred for use as passivation elements, such as for color conversion.
In the example of
In some cases, transferring the heterostructure or a portion thereof may include an act 630 in which the transferred portion is mechanically exfoliated. In some cases, the mechanical exfoliation may be performed on the as-grown GaN quantum dot structures using polyimide tape. In one example involving GaN quantum dots on a triangular hBN flake, all of the quantum dots were exfoliated, thereby confirming the weak van der Waals interaction between the GaN quantum dots and the hBN flake. The mechanical exfoliation exclusively removes the GaN quantum dots without affecting the underlying 2D hBN flake. Further details regarding the exfoliation are provided below in connection with
The heterostructure or quantum dot structures may be transferred to the device substrate in an act 632. In such cases, the heterostructure or quantum dot structures exhibit bonding with the device substrate via van der Waals forces. For instance, the semiconductor material of the quantum dot structures may exhibit bonding with the device substrate via van der Waals forces. The heterostructure or quantum dot structures may thus be in contact with the device substrate. The manner in which the transfer is achieved may thus vary, e.g., in connection with the composition and/or other characteristics of the device substrate.
The method 600 may include one or more additional acts. For instance, one or more acts may be configured or directed to forming additional layers of the heterostructure or other structures of the device. In some cases, one or more metal layers may be deposited and patterned to form one or more contacts or electrodes.
The method 600 may include fewer, alternative, or additional acts. For example, the method 600 may include the implementation of one or more doping procedures for one or more of the semiconductor elements described herein. Such doping may be useful in connection with charge carrier confinement and/or other purposes. The method 600 may also include any number of additional acts directed to forming additional layers of the heterostructure or other structures of the device. In some cases, one or more metal layers may be deposited and patterned to form one or more contacts or electrodes.
As shown in part (b) of
The exfoliation allows free-standing quantum dot structures and subsequent transfer to other functional substrates. Such transfer may be used to form a variety of integrated optoelectronic and quantum devices.
With reference again to part (d) of
The device 100 includes a substrate 104 and a heterostructure 102 supported by the substrate 104. The heterostructure 102 includes a set of quantum dot structures (or nanocrystals) 106. In the example of
The substrate 104 may be composed of, or otherwise include, nickel, but alternative or additional materials may be used, including for instance, graphene or graphite. In this example, the heterostructure 102 is in contact with the substrate 104. In other cases, one or more layers are disposed between the substrate 104 and the heterostructure 102.
The heterostructure 102 further includes a layered material 108 disposed between the set of quantum dot structures 106 and the substrate 104. The layered material 106 includes a plurality of monolayers 108 such that adjacent monolayers 108 of the plurality of monolayers are bonded to one another via van der Waals forces, and such that the semiconductor material of each quantum dot structure (or nanocrystal) 106 of the set of quantum dot structures (or nanocrystals) exhibits bonding with the layered material via van der Waals forces. In the example of
In some cases, the substrate 104 is composed of, or otherwise includes, a covalently bonded material. In such cases, the layered material 108 has a number of monolayers 110 sufficient to screen the set of quantum dot structures (or nanocrystals) 106 from a potential field of the covalently bonded material. Accordingly, and as described herein, each quantum dot structure (or nanocrystal) 106 of the set of quantum dot structures (or nanocrystals) may be bonded to one of the plurality of monolayers 110 via van der Waals forces. The heterostructure 102 thus lacks a wetting layer (e.g., a wetting layer between the quantum dot structures 106 and the substrate 104). The quantum dot structures (or nanocrystals) 106 may also thus exhibit multiple crystallographic orientations.
In the example of
In some cases, the substrate 104 of the device 100 may correspond with a device substrate to which the heterostructure 102 (or a portion thereof) has been transferred, as described above. For example, the quantum dot structures 106 may be transferred to a device substrate. As a result, the quantum dot structures 106 may be in contact with the substrate 104. As described above, the substrate 104 may exhibit one or more properties (e.g., conductive, transparent, etc.) in support of the device functionality.
Described above are examples of methods and devices involving a new class of QD heterostructures that overcome the fundamental limitations of current approaches to QD formation. Such current approaches generally involve the use of etching, Stranski-Krastanov (SK) growth mode, or solution processing, each of which exhibit very limited material quality. For example, SK QD formation is driven by the large lattice mismatch between the QD active region and the underlying substrate, resulting in the formation of a two-dimensional wetting layer as well as interfacial defects and large size dispersion, which severely limits the application of QDs. By utilizing hexagonal boron nitride (hBN) as a supporting material or substrate, the disclosed methods are capable of forming van der Waals GaN quantum dots without the presence of a two-dimensional wetting layer. Moreover, the GaN QDs are free of dislocations and stacking faults due to the van der Walls interfacial interaction. Compared to GaN QDs formed on AlN or Si substrates, van der Waals QDs grown on hBN monolayers exhibit drastically improved optical quality. For instance, the photoluminescence emission intensity for examples of QDs on hBN was four times stronger despite having a QD density nearly two orders of magnitude lower. Enhanced growth duration further leads to the formation of GaN nanocrystals, which show multiple crystallographic orientations through vdW interactions. The disclosed devices and methods accordingly provide a new strategy for synthesizing high quality QD structures, which, in turn, support or enable next-generation high performance optoelectronic and other quantum devices.
The present disclosure has been described with reference to specific examples that are intended to be illustrative only and not to be limiting of the disclosure. Changes, additions and/or deletions may be made to the examples without departing from the spirit and scope of the disclosure.
The foregoing description is given for clearness of understanding only, and no unnecessary limitations should be understood therefrom.
This application claims the benefit of U.S. provisional application entitled “van der Waals Quantum Dots,” filed Mar. 16, 2022, and assigned Ser. No. 63/320,462, the entire disclosure of which is hereby expressly incorporated by reference.
This invention was made with government support under Contract No. 2118809 awarded by the National Science Foundation. The government has certain rights in the invention.
Filing Document | Filing Date | Country | Kind |
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PCT/US2023/015378 | 3/16/2023 | WO |
Number | Date | Country | |
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63320462 | Mar 2022 | US |