The present invention relates to surface emitting laser, and more particularly, relates to two-dimensional material plasmonic laser.
Monolayer transition metal dichalcogenides (TMDCs) are promising materials for light-emitting devices because they change from indirect to direct band-gap semiconductors when passing from the multilayer (bulk) to the monolayer regime1. One import recent development for such devices is the demonstration of lasing by coupling monolayer TMDC gain media with high-quality-factor (high-Q, Q≈1,000-5,000) photonic cavity modes2-4, such as defect modes in photonic crystals2, 4 and whispering-gallery modes in a microdisk3. However, the two-dimensional (2D) nature of monolayer TMDCs has not been fully explored in these photonic-cavity lasers. Especially, monolayer TMDCs could open up new possibilities for semiconductor surface-emitting lasers, which are efficient in light extraction and can be used to fabricate 2D microlaser arrays with low lasing threshold5 for applications in high-speed optical communications, displays, lighting, sensing, and imaging. At present, the performance of surface-emitting lasers is limited by viable semiconductor heteroepitaxial growth, especially for the visible and long infrared spectral ranges. In contrast, the surfaces of the van der Waals monolayers (TMDCs, graphene, hexagonal boron nitride) are naturally passivated, leading to exceptional versatility in device fabrications such as formation of heterostructures via stacking and easy integration with dissimilar materials (metals, oxides, etc.).
A vertical-cavity surface-emitting laser (VCSEL) is a type of semiconductor laser diode with laser beam emission perpendicular from the top surface. The laser resonator of the vertical-cavity surface-emitting laser consists of two distributed Bragg reflector (DSR) mirrors parallel to the wafer surface with an active region consisting of one or more quantum wells for the laser light generation in between. The planar DBR-mirrors consist of layers with alternating high and low refractive indices. Each layer has a thickness of a quarter of the laser wavelength in the material. At present, the poor optical, electrical, and thermal properties of available DBR mirror materials hinder the realization of VCSELs to be used over a broad spectrum, especially for the visible and long infrared spectral ranges, severely limiting their potential applications.
To realize monolayer semiconductor surface-emitting lasers, the 2D geometry and in-plane orientation of exciton dipole moment call for an optimized design of laser cavity. Metal-based surface plasmon polariton (SPP) cavities are particularly attractive because they can concentrate the propagating SPP waves along the metallodielectric interface, allowing a near-field coupling to the tightly confined exciton transition dipole moments. Such advantages have been recognized immediately after the inception of monolayer TMDCs as an emerging 2D photonic materials6. Indeed, orders of magnitude enhancement in photoluminescence (PL) has been reported in a recent work7. However, plasmonic-cavity-enabled lasing has not yet been realized because of stringent requirements in low-loss plasmonic material and cavity design.
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In one general aspect, the present invention relates to surface emitting laser, and more particularly, relates to two-dimensional material plasmonic laser.
According to an embodiment of this invention, a two-dimensional material plasmonic laser is provided with a surface plasmonic cavity and an atomically thin semiconductor monolayer gain medium disposed on the surface plasmonic cavity. Under optical pumping or electrical pumping, the surface plasmonic cavity provides a laser feedback mechanism by coupling electron-hole pairs confined in the atomically thin semiconductor monolayer gain medium and surface plasmon modes in the surface plasmonic cavity, and a laser light is emitted from the two-dimensional material plasmonic laser.
In an embodiment, the laser light is emitted in a direction normal to the atomically thin semiconductor monolayer gain medium. In an embodiment, the plasmonic resonance wavelength of the surface plasmonic cavity can be tuned across the complete visible and infrared spectral range.
In an embodiment, the atomically thin semiconductor monolayer gain medium is a transition metal dichalcogenide monolayer with a formula MX2, where M is a transition metal atom and X is a chalcogen atom. In an embodiment, the surface plasmonic cavity is composed of near-field coupled plasmonic structures. In an embodiment, the surface plasmonic cavity has a configuration comprising nanogroove gratings, spiral gratings, line patterns, dot patterns, or concentric circles.
In an embodiment, the plasmonic resonance wavelength is determined by structure parameters of the surface plasmonic cavity. In an embodiment, the surface plasmonic cavity is a nanogroove grating, and the plasmonic resonance wavelength is determined by the groove width, depth, and/or pitch of the nanogroove grating. In an embodiment, the surface plasmonic cavity is a nanogroove grating with different widths and/or depths resulting in multiple plasmonic resonances.
In an embodiment, the surface plasmonic cavity is made of silver, aluminum, gold, boron nitride, titanium nitride, graphene, or combinations thereof. In an embodiment, a strongly coupled resonance energy transfer between the surface plasmon mode and the electron-hole pairs (excitons) leading to an energy level splitting (Rabi splitting) and formation of upper (UP) and lower (LP) exciton-polaritons. In an embodiment, the laser light has a lasing linewidth less than 1 nm. In an embodiment, upper thin-film electrodes are further arranged on the atomically thin semiconductor monolayer gain medium in case of the electrical pumping. In an embodiment, one top electrode is further arranged on the atomically thin semiconductor monolayer gain medium for applying voltage versus the surface plasmonic cavity. In an embodiment, the surface plasmonic cavity comprises a pair of surface mirrors.
The success demonstration of small-footprint, open-geometry surface emitting lasers based on two-dimensional material device architectures can bring about significant advancement in integrated photonic technologies.
Reference will now be made in detail to specific embodiments of the invention. Examples of these embodiments are illustrated in accompanying drawings. While the invention will be described in conjunction with these specific embodiments, it will be understood that it is not intended to limit the invention to these embodiments. On the contrary, it is intended to cover alternatives, modifications, and equivalents as may be included within the spirit and scope of the invention as defined by the appended claims. In the following description, numerous specific details are set forth in order to provide a thorough understanding of the present invention. The present invention may be practiced without some or all of these specific details. In other instances, well-known process operations and components are not described in detail in order not to unnecessarily obscure the present invention. While drawings are illustrated in details, it is appreciated that the quantity of the disclosed components may be greater or less than that disclosed, except expressly restricting the amount of the components. Wherever possible, the same or similar reference numbers are used in drawings and the description to refer to the same or like parts.
Referring to
To realize 2D monolayer semiconductor surface-emitting lasers, here a preferred embodiment is proposed and demonstrated with a low-loss feedback mechanism based on surface plasmon polariton (SPP) cavities with unique coupling properties in both real- and momentum-space. In this cavity design, the SPP modes on metallic surface cavities allows for efficient 2D feedback schemes by concentrating the optical field into a subwavelength region with an enhanced in-plane field component for strong light-gain-medium interactions. Furthermore, the dark SPP modes trapped in the case of dark SPP resonators do not couple to the optical far-field, significantly reducing the radiative damping.
Plasmonic material losses in the SPP cavities are typically very high (Q<100). The embodiments of this invention use atomically smooth, single crystalline silver (Ag) as a low-loss plasmonic platform and demonstrate lasing from monolayer TMDC using two different SPP cavity designs. The adoption of surface plasmonic cavities represents a significant paradigm shift of 2D material lasers, which offer unique advantages such as subdiffraction integration and facile spectral/spatial matching with the monolayer gain medium. In comparison to the photonic counterpart, the strongly enhanced optical field and light-matter interactions in the plasmonic cavity greatly alleviate the high-Q requirement.
Plasmonic-Cavity Surface-Emitting Laser
The concept of 2D material surface-emitting laser (plasmonic-cavity surface-emitting laser, PCSEL) is schematically shown in
As the optical gain media for surface-emitting lasers, the TMDC monolayers have the advantage of exhibiting strong excitonic effects, originated from unusually large exciton binding energies in reduced dimensionality10,11. Moreover, their large exciton oscillator strengths (fosc) can lead to large optical absorption coefficients and strong light-matter interaction (∞√{square root over (fosc)}). Indeed, strong coupling of exciton and cavity photon/plasmon with large Rabi splitting ranging from a few tens to ˜100 meV has been demonstrated for TMDC monolayers12-15. In principle, the exciton-cavity coupling strength is proportional to √{square root over (N/Vm)}, where N is the number of emitters coupled to the cavity mode volume Vm16-18. Thus, the ultrasmall plasmonic mode volume19-21 is particularly promising to realize strong light-matter interaction using atomically thin semiconductor media. In addition, monolayer TMDCs are excellent materials as the gain media for surface-emitting plasmonic lasers with a versatile 2D open-cavity configuration, enabling easy access to the plasmonic mode volume in which the optical processes take place.
Despite their tremendous potential, plasmonic lasers based on 2D materials are yet to be demonstrated. By adopting the spaser concept22-30 with a metal-insulator-semiconductor plasmonic structure23-25, here the inventers succeed in realizing the continuous-wave (CW) operation of TMDC monolayer-based PCSELs with low lasing thresholds. The key behind this success lies in the design of plasmonic cavities consisting of nanogroove gratings, which can be precisely fabricated by focused ion beam (FIB) milling31. Also, large single-crystalline Ag colloidal crystals were utilized to obtain ultra-long SPP propagation length and low-loss exciton-SPP coupling32, 33. After FIB milling, conformal Al2O3 layers (˜5 nm in thickness) were deposited using the atomic layer deposition (ALD) method to protect the Ag plasmonic cavities and to prevent photoluminescence (PL) quenching of deposited WS2 monolayers.
The exciton-cavity coupling strength is very sensitive to the relative orientation of the cavity electric field and the dipole moments of excitons in TMDC monolayers, which have an in-plane orientation12, 34. In the photonic Fabry-Perot (FP) cavity, the strong interaction occurs at the antinode plane parallel to the distributed Bragg reflector mirrors12. For the plasmonic cavity, the electric field also needs to be in a plane parallel to the monolayer to facilitate effective coupling to excitons. The FDTD simulations shown in
Surface Plasmonic Cavity
In the embodiments of this invention, the formation of dark (subradiative) and bright (radiative) modes in the Ag nanogroove cavities involves two different coupling mechanisms: (1) near-field plasmonic coupling35, 36 of individual nanogroove modes, and (2) far-field diffractive coupling37 of nanogroove modes and the grating mode. In both cases, the plasmonic resonance and dispersion of Ag nanogroove cavity can be precisely controlled by proper choice of the groove width (w), depth (d), and/or pitch (p).
To understand the coupling behavior of nanogroove arrays, the reflectance spectra of nanogroove arrays were measured with continuously varying pitches using angularly and spectrally resolved mapping via a back-focal-plane imaging technique31. For the optical reflectance measurements, the reflected light of a halogen lamp was collected through a polarizer so that the electric field is parallel to the grating vector [i.e., horizontal (H)-polarization]. All measurements were performed with the spectrometer entrance slit perpendicular to the grating nanogrooves.
In the case of near-field coupling, the localized plasmonic resonance of individual nanogrooves can be controlled by nanogroove width/depth38 and it is sensitive to the change of local dielectric environment (
On the other hand, the far-field radiation of bright cavities (p=360 to 620 nm) originates from in-plane diffractive orders grazing to the plane of nanogroove grating (i.e., Wood's anomalies shown as purple dashed lines using the effective index of SPP wave propagating on the Al2O3-protected Ag surface32. In the angle-resolved reflectance spectra, mode anticrossing and splitting37 due to strong coupling between nanogroove and grating modes can be clearly observed and the resulting coupling is highly directional, as evidenced by the presence of a large Rabi splitting (˜370 meV) at the Γ point.
Strong Exciton-SPP Coupling
To date, surface plasmonic lattice lasers26-29 and 2D distributed Bragg feedback lasers40 reported in the literature are based on the far-field diffractive coupling mechanism, which can lead to lasing action at the band edges. However, as the diffractive coupling is through a limited region in the momentum space (k-space), the coupling efficiency might not be sufficient for an atomically thin gain medium. Here, the embodiments of this invention utilize the dark-mode surface plasmonic cavities for the realization of 2D exciton-polariton lasing. The flattened SPP band and large group index in these cavities enable efficient coupling with the atomically thin gain medium.
The black resonance curves in
In the double-resonant cavity structure shown in
The dispersionless dark cavity mode enables an efficient coupling with monolayer WS2 in a wide range of k-space. Indeed, the angle-resolved reflectance mapping measured for a monolayer WS2 integrated onto a double-resonant cavity with resonances at the XA and XC resonances (FIG. 3, c and d) confirm that a uniform Rabi splitting at the XA resonance occurs across a wide range of incident angles except slight deviation at large angles due to the interaction with the grating mode. Because of the angle-insensitive strong coupling, the resulting upper (UP) and lower (LP) exciton-polariton bands are also close to flat bands in a wide range of k-space (
Lasing Characteristics
Using the dark-mode concept, the inventors have been able to demonstrate two different monolayer WS2 plasmonic lasers. A second embodiment of this invention is the simplest design, in which a surface FP cavity uses a pair of lateral reflectors (the single-resonant structure shown in
The inventors found that the lasing mode is at 628 nm, corresponding to one of the two surface FP cavity modes observed in the optical scattering spectra (
In comparison, using the double-resonant plasmonic cavity structure shown in
By fitting the experimental data using laser rate equations, a spontaneous-emission coupling factor (β) of 0.08 and an ultralow lasing threshold of 100 W/cm2 (
Besides the low lasing threshold, another important advantage of lasing under strong coupling is that very narrow emission linewidth can be obtained using a low-Q laser cavity. The initial PL linewidth from polaritonic emission is already rather narrow (˜2.5 nm). Above the lasing threshold, the inventors have confirmed the concurrence of further linewidth narrowing (˜0.8 nm at high pumping power) and nonlinear growth of emission intensity with increasing excitation (
In summary, the strong oscillator strength of TMDC monolayer and the ultrasmall mode volume of Ag surface plasmonic cavity jointly form an ideal hybrid material platform to realize 2D material surface emitting lasers. The dark SPP cavities are advantageous due to a 2D feedback mechanism with high coupling efficiency and low radiative loss. Using Fourier-plane mapping, the inventors have confirmed that coupling to dark propagating SPP modes in surface cavities occurs in a wide range of momentum space. The successful demonstration of surface exciton-polariton lasing opens a unique way to coherently manipulate the light-matter interaction on plasmonic metal surfaces, offering the promise of new scientific discoveries and photonic applications.
The following supplementary information describes materials and methods for forming and measuring a two-dimensional material plasmonic laser according to the preferred embodiment of this invention. While embodiments of the present invention are described with specific regard to dichalcogenide (TMDC) mamolayers, it is to be appreciated that embodiments of the invention are not so limited and that certain embodiments may also be applicable to other two-dimensional material monolayers such as allotropes of phosphorus (e.g., black phosphorus), 2D group-IV materials, 2D group-V materials, 2D oxides, and graphene oxide monolayers.
Colloidal Silver (Ag) Crystals
Colloidal silver single crystals were synthesized by using a platinum (Pt)-nanoparticle-catalyzed and ammonium hydroxide (NH4OH)-controlled polyol reduction method32. By controlling the concentration of ammonium hydroxide, millimeter-sized single-crystalline silver plates can be grown at room temperature.
Fabrication of Nanogroove Grating Structures
Both single- and double-resonant surface plasmonic cavity structures on colloidal Ag single crystals were fabricated by using a focused ion beam (FIB) system (FEI Helios Nanolab 600i). These structures were milled at a 30-kV acceleration voltage and with an ion beam current of 1.2 pA. After the FIB fabrication, surface cavity structures were immediately capped with a 5-nm-thick Al2O3 conformal layer through an atom layer deposition (ALD) system.
Optical Setups for Reflectance Measurements at Room Temperature
The reflectance spectra measured for the nanogroove grating structures at room temperature were acquired by using a white light source (halogen lamp) at normal incident through a 100x objective lens (Olympus, N.A.=0.8) and a polarizer. The direction of polarizer is perpendicular to the nanogrooves (parallel to the grating vector). The reflection light was collected by the same objective lens and dispersed by a spectrometer (Andor, Shamrock 500i) equipped with a thermoelectrically cooled charge-coupled device (CCD) detector.
Optical Dark-Field Imaging
The reflected dark-field and bright-field images were acquired by using a Zeiss optical microscope. The silver grating samples were excited by a halogen lamp through a 100x (N.A.=0.75) objective lens and the scattered/reflected light was collected by the same objective lens.
Measurements of Lasing and Reflectance Characteristics at Cryogenic Temperatures
Low-temperature PL and lasing measurements were performed by using a low-vibration, closed-cycle cryostats system (attocube, AttoDRY800) with a 100× objective lens (attocube, LT-APO/VIS, N.A.=0.82) inside the vacuum chamber. A continuous-wave (CW) green semiconductor diode laser at 532 nm was used as the optical excitation source with a spot size about 2 μm. The optical excitation and collection of emission from the cavity structures were carried out using the same objective lens at normal incidence, and the emission signal was dispersed by a homebuilt spectrometer equipped with a TE-cooled CCD (Andor, iDus 420). Moreover, reflectance measurements were carried out by the same system except that a halogen lamp was used as the excitation white light source.
FDTD Simulations
The inventors used a commercial FDTD package (Lumerical Solutions) to simulate the cavity properties. In these simulations, the dielectric functions of the composing materials were obtained from the following sources: the dielectric function of silver single crystal was adopted by using the experimental data for an epitaxial silver film44; the refraction index of Al2O3 is assumed to be 1.77; and the dielectric function of WS2 monolayer was adopted by using a published experimental data set45.
2D Plasmonic Cavity
The surface plasmonic cavity was designed using the concept of dark propagating modes via near-field coupling. There are much less radiation losses in a dark mode, in comparison to the bright mode case36.
Angularly and Spectrally Resolved Reflectance Measurements
Strong exciton-polariton coupling is essential to achieve CW, low-threshold lasing (˜100 W/cm2) using a single monolayer TMDC gain medium. Dispersion relations measured by angle-resolved spectroscopy allow one to characterize the strong coupling phenomenon. In
In the case of far-field, diffractive coupling, the dispersions of diffracted orders (grating modes) can be expressed by using the grating equation (Wood's anomalies): kd,∥=ki,∥±Gm, where ki,∥ is incident wave vector
angular frequency and speed of incident light in free space; θ: incident polar angle (θ=0 for normal incidence); êi: in-plane unit vector along the incident direction], kd,∥ is the diffracted wave vector
effective index defining the phase velocity of the diffracted wave, including the far-field radiation into air from photons (photonic mode, neff=nair) and the propagating SPPs (plasmonic mode, neff=nSPP) on the Ag surface; êd: in-plane unit vector along the diffracted direction], and
is the grating vector (the reciprocal lattice vector; m: integer number; in-plane unit vector perpendicular to the grating nanogrooves). It is important to recognize that Wood's anomalies are highly directional, which only can be coupled to a limited region of the momentum space (k-space). For the nanogroove gratings, using the incident excitation geometry described in terms of polar (θ) and azimuthal (ϕ; ϕ=0 for incidence light along the {circumflex over (x)} direction) angles, the Bragg scattering condition requires that kd,∥2=ki,∥2+Gm2±2ki,∥Gm cos(ϕ). In comparison with the plasmonic cavity under the near-field coupling conditions, the far-field-coupled plasmonic cavity (pitch=600 nm, bright mode) [Note: for simplicity, the nanogroove width and depth were fabricated to exhibit plasmonic resonance in the infrared region (outside the measured spectral range)] has a limited region of momentum space (near the Γ point of k-space) interacting strongly with the excitonic resonance of WS2 monolayer. For this nanogroove grating, the dispersion relations of the SPP modes propagating along the nanogroove grating (ϕ=0°) are defined by the phase matching condition shown below
where ki,∥=ki sin(θ)=(ω/c)sin(θ) is the in-plane wave vector of the incident light, p is the grating pitch, m is an integer, and neff is effective index defining the phase velocity of the diffracted wave, including the far-field radiation from photons (photonic mode, neff=pair=1) and propagating SPPs on the Ag surface (plasmonic mode, neff=nSPP=[(εAgεair)/(εAg+εair)]1/2, where εAg is the silver dielectric function). Thus, the dispersion relations resulting from the first-order TM modes (ϕ=0°, m=±1) can be expressed as
Substituting the experimental SPP dispersion data (neff) on an Al2O3 (5 nm)-protected Ag surface32 into these formulas, the SPP dispersion curves (yellow dashed lines) can be obtained, which are in excellent agreement with our previous experimental results. This indicates that the far-field-scattered plasmonic mode contributes more to the measured reflectance and the effective index of SPPs propagating on the Ag nanogroove grating surface is close to those propagating on the unpatterned Ag surface. In the cases of first-order normal-incidence modes (θ=0° and m=±1), the mode wavelength can be simplified to λ=neff·p, where λ is λair (photonic modes) or λSPP (plasmonic modes). For the photonic modes (neff=nair=1), the first-order modes intercept at λ=nair·p=p (600 nm).
Low-Temperature Reflectance Measurement
At 8K, the A-exciton peak of WS2 shifts to 585 nm (
The intent accompanying this disclosure is to have each/all embodiments construed in conjunction with the knowledge of one skilled in the art to cover all modifications, variations, combinations, permutations, omissions, substitutions, alternatives, and equivalents of the embodiments, to the extent not mutually exclusive, as may fall within the spirit and scope of the invention. Corresponding or related structure and methods disclosed or referenced herein, and/or in any and all co-pending, abandoned or patented application(s) by any of the named inventor(s) or assignee(s) of this application and invention, are incorporated herein by reference in their entireties, wherein such incorporation includes corresponding or related structure (and modifications thereof) which may be, in whole or in part, (i) operable and/or constructed with, (ii) modified by one skilled in the art to be operable and/or constructed with, and/or (iii) implemented/made/used with or in combination with, any part(s) of the present invention according to this disclosure, that of the application and references cited therein, and the knowledge and judgment of one skilled in the art.
Conditional language, such as, among others, “can,” “could,” “might,” or “may,” unless specifically stated otherwise, or otherwise understood within the context as used, is generally intended to convey that embodiments include, and in other interpretations do not include, certain features, elements and/or steps. Thus, such conditional language is not generally intended to imply that features, elements and/or steps are in any way required for one or more embodiments, or interpretations thereof, or that one or more embodiments necessarily include logic for deciding, with or without user input or prompting, whether these features, elements and/or steps are included or are to be performed in any particular embodiment.
All of the contents of the preceding documents are incorporated herein by reference in their entireties. Although the disclosure herein refers to certain illustrated embodiments, it is to be understood that these embodiments have been presented by way of example rather than limitation. For example, any of the particulars or features set out or referenced herein, or other features, including method steps and techniques, may be used with any other structure(s) and process described or referenced herein, in whole or in part, in any combination or permutation as a non-equivalent, separate, non-interchangeable aspect of this invention. Corresponding or related structure and methods specifically contemplated and disclosed herein as part of this invention, to the extent not mutually inconsistent as will be apparent from the context, this specification, and the knowledge of one skilled in the art, including, modifications thereto, which may be, in whole or in part, (i) operable and/or constructed with, (ii) modified by one skilled in the art to be operable and/or constructed with, and/or (iii) implemented/made/used with or in combination with, any parts of the present invention according to this disclosure, include: (I) any one or more parts of the above disclosed or referenced structure and methods and/or (II) subject matter of any one or more of the inventive concepts set forth herein and parts thereof, in any permutation and/or combination, include the subject matter of any one or more of the mentioned features and aspects, in any permutation and/or combination.
Number | Name | Date | Kind |
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20170338621 | Li | Nov 2017 | A1 |
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