Interface and surface engineering of black phosphorus: a review for optoelectronic and photonic applications
doi: 10.1088/2752-5724/ac49e3
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Abstract: Since being rediscovered as an emerging 2D material, black phosphorus (BP), with an extraordinary energy structure and unusually strong interlayer interactions, offers new opportunities for optoelectronics and photonics. However, due to the thin atomic body and the ease of degradation with water and oxides, BP is highly sensitive to the surrounding environment. Therefore, high-quality engineering of interfaces and surfaces plays an essential role in BP-based applications. In this review, begun with a review of properties of BP, different strategies of interface and surfaces engineering for high ON-OFF ratio, enhanced optical absorption, and fast optical response are reviewed and highlighted, and recent state-of-the-art advances on optoelectronic and photonic devices are demonstrated. Finally, the opportunities and challenges for future BP-related research are considered.
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Key words:
- black phosphorus /
- interface engineering /
- surface engineering /
- optoelectronics /
- photonics
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Figure 1. Lattice and electronic band structures of BP. (a) Schematic illustration of the puckered lattice structure of BP. Reprinted from [20] by permission from Springer Nature Customer Service Centre GmbH. (b) Brillouin zone of the primitive cell of BP.(c) Electronic band structure for BP by the mBJ potential (dashed blue line) and the HSE06 functional (solid red line) calculations, respectively. The zoom-in plot in the right of the figure shows the bandgap of BP at z point. (b) and (c) are reprinted from [16] by permission from Springer Nature Customer Service Centre GmbH. (d), (e) Band structures of monolayer (d) and bilayer BP (e), which are calculated by the tight-binding parametrization. Reprinted with permission from [68], copyright (2014) by the American Physical Society.
Figure 2. Optical properties of BP. (a) The tunable optical energy gap of multilayer BP with different thicknesses. Reprinted with permission from [18], copyright (2014) by the American Physical Society. (b), (c) Optical absorption spectra for the incident light with the polarization direction along armchair (b) and zigzag (c) directions. The thicknesses of BP vary from one layer to five layers. Reprinted from [16] by permission from Springer Nature Customer Service Centre GmbH. (d)-(g) Exciton effects as well as exciton binding energies in BP. (d) Optical transitions between two quantized sub-bands of BP, based on the quasi-one-dimensional tight-binding model. (e) The model of optical absorption of few-layer BP when considering the exciton resonances, including exciton ground (1s), excited (2s) states, and continuum (step-like) states. Reprinted from [22] by permission from Springer Nature Customer Service Centre GmbH. (f) Real part of the optical conductivity of 6L BP on a quartz substrate with incident light polarizations from 15 to 90. (g) Theoretical values of exciton binding energies of free-standing BP (black dots) and BP (red dots) on the PDMS substrate, respectively. (f) and (g) are reproduced from [77], CC BY 4.0. (h)-(j) Plasmons in BP. (h) Calculated energy loss dispersion for electron doping in BP of 1 1013 cm-2 and momentum q paralleled with x (right) and y (left) directions, respectively. (i) Scaling of plasmon frequency with electron concentration of monolayer and 20 nm thick BP, where graphene is for comparison. (j) Distribution of anisotropic plasmons in k surface. (h) and (i) are reprinted with permission from [78], copyright (2014) by the American Physical Society. (j) is reprinted with permission from [68], copyright (2014) by the American Physical Society.
Figure 3. Nonlinear optics in BP. (a), (b) Third-harmonic generation (THG) in a multilayer BP flake. Reprinted with permission from [89], copyright (2017) American Chemical Society. (a) Optical image of the BP flake. (b) THG mapping image excited by a 1557 nm pump laser. (c) Nonlinear refractive index n2(
) of BP along the armchair direction by the numerical simulation, demonstrating the Kerr nonlinearity. Reproduced from [92]. © IOP Publishing Ltd. All rights reserved. (d)-(e) Nonlinear optical absorption of BP. Reprinted with permission from [93], copyright (2016) American Chemical Society. (d) Normalized differential absorptivity of BP, graphene and MoS2 nanosheets under different incident light fluence. (e) The values of the imaginary part of the third-order nonlinear optical susceptibility Im (3) of BP and graphene measured at different light wavelengths. (f) Transient absorption curve of the BP dispersion at 1550 nm, where the inset illustrates the dynamic carrier process. Reproduced with permission from [48], John Wiley & Sons [© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim]. 
Figure 4. Degradation of BP. (a), (b) AFM image of BP immediately exfoliated on the SiO2 substrate (a) and placed under ambient conditions after a few days (b). Reprinted from [104] by permission from Springer Nature Customer Service Centre GmbH. (c) Schematic illustration of the light-induced ambient degradation mechanism of BP. Reproduced with permission from [102], John Wiley & Sons [© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim]. (d)-(f) Degradation-induced changes in optical absorption spectra as well as electronic band structures of BP. (d), (e) Blueshift of exciton resonances of 3 L (d) and 8 L (e) BP. (f) Changes of E11 and E22 peak energies as function with exposure time at the ambiance of 8 L BP. Reprinted with permission from [105], copyright (2019) by the American Physical Society.
Figure 5. (a)-(c) Schematic diagrams of Homojunctions based on BP. (a) A vertical BP p-n homo-structure based on a typical ionic gel gating configuration. Reprinted from [30] by permission from Springer Nature Customer Service Centre GmbH. (b) A lateral BP p-n structure by chemical doping methods, where Al2O3 is the surface hole dopant and BV is the surface electron dopant. Reprinted from [58], copyright (2016), with permission from Elsevier. (c) A trilayer homo-structure based on three BP flakes with orthogonally crystal directions. Reprinted from [109] by permission from Springer Nature Customer Service Centre GmbH. (d)-(i) Schematic diagrams of three different BP-semiconductor heterojunctions and the corresponding energy structures. (d), (g) BP-WSe2 Type-I heterojunction. Reproduced from [113]. CC BY 4.0. (e), (h) BP-MoS2 Type-II heterojunction. Reprinted from [29] by permission from Springer Nature Customer Service Centre GmbH. (f), (i) BP-ReS2 Type-III heterojunction. Reprinted with permission from [114], copyright (2019) American Chemical Society.
Figure 6. Exciton generation, dissociation, and harvesting mechanisms in BP-semiconductor heterostructures. (a)-(c) Exciton dissociation at the interface of BP/P3HT and the enhancement of photocurrent generation. Reprinted with permission from [115], copyright (2019) American Chemical Society. (a) Schematic diagram of the transfer of electrons and holes at the BP/P3HT interface. (b) Migration of electrons and holes adjacent to the p-n heterojunction. (c) I-V characteristics of BP (left) and BP/P3HT heterostructure (right) under dark and 650 nm light illumination conditions reflect the enhancement of photocurrent in the heterostructure. (d)-(f) Multiple exciton generation and harvesting in BP-MoS2 heterostructure. Reprinted with permission from [116], copyright (2020) American Chemical Society. (d) Theoretically calculated band alignment indicates the generation of multiple excitons from 4 L BP and the exciton dissociation by interfacial electron transfer to MoS2. (e) Transient optical absorption spectra of heterostructure under 1.36 eV excitation. (f) Transient absorption kinetics of MoS2 A exciton within 1.5 ps time scale under 1.36 and 2.25 eV excitation energies, respectively.
Figure 7. Interface engineering between BP and metals. (a), (b) Ni/Au and Pd/Au contacts depositing on BP flakes. Reprinted with permission from [122], copyright (2014) American Chemical Society. (a) Schematic illustration. (b) Contact resistance characteristics with different back-gate voltage. (c), (d) Graphene as electrodes for BP functional layer. Reprinted with permission from [46], copyright (2020) American Chemical Society. (c) Schematic illustration of a BP flake sandwiched by two graphite films. (d) Typical I-V characteristics of the graphite-BP-graphite device. (e), (f) Metals on BP for light-matter interaction enhancement. Reprinted with permission from [126], copyright (2021) American Chemical Society. (e) T-shaped Au nano-antennas with polarization-tailoring alignments on BP. (f) Enhanced optical absorption of BP for x- and y-polarized light incidence.
Figure 8. Interface engineering between BP and dielectric materials. (a) and (b) BP between oxide and air layers as natural quantum wells for electro-optical effects [33, 133]. (a) Schematic diagram of a BP flake on SiO2 substrate as a gate-tunable device for electro-optical effects. Reprinted with permission from [133], copyright (2017) American Chemical Society. (b) Energy band structure illustrating the change of bandgap of BP natural quantum wells under intrinsic, QCFK, and BMS regimes, respectively. Reprinted with permission from [33], copyright (2016) American Chemical Society. (c) Schematic diagram of BP sandwiched by two hBN layers. Reprinted from [135] by permission from Springer Nature Customer Service Centre GmbH. (d) Exciton characteristics including quasi-particle gaps, optical gaps, and binding energy in 1-4 L BP with and without dielectric encapsulation. Reprinted with permission from [60], copyright (2017) American Chemical Society.
Figure 9. Surface engineering of BP. (a), (b) Al-doped BP as n-doped functional layers for transistor characterizations. Reproduced with permission from [42], John Wiley & Sons. [© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim]. (a) Schematic diagram that shows Al atoms as electron dopants for the BP host lattice. (b) Transfer characteristics of BP transistors, which indicate the transform from p-type to n-type of BP when doping Al atoms. The inset is the same plotted data but using a logarithmic scale. (c) Energy band alignment of BP and BV, which exhibits the n-type chemical doping effect of few-layer BP. Reprinted from [58], copyright (2016), with permission from Elsevier. (d)-(f) Oxidation and surface coating for ambiently stable BP. Reproduced from [146]. CC BY 4.0. (d) O2 plasma etching and Al2O3 coating on a BP flake. (e) Optical images of fresh exfoliated (left) and O2 plasma etched (middle) BP, as well as the PL mapping image. (f) Visual images of an O2 plasma etched BP flake before and after three days and a PxOy + Al2O3 coated BP flake before and after 30 days.
Figure 10. Interface and surface engineering of BP for optoelectronic applications. (a), (b) BP vertical p-n junction-based photodetector with polarization sensitivity. Reprinted from [30] by permission from Springer Nature Customer Service Centre GmbH. (a) Optical microscope image of the device that a ring-shaped Ti/Au electrode is applied to avoid the extra polarization originating from the straight edge of the metal. (b) Photocurrent mapping images of the BP inside the ring electrode under a linear-polarized light with the polarization direction from 0 to 90. (c)-(e) A concept of proof of a BP-based MIR spectrometer. Reprinted from [162] by permission from Springer Nature Customer Service Centre GmbH. (c) Schematic illustration of the hBN/BP/hBN heterostructure-based spectrometer. (d) An array of source-drain current with different values of the top-gate (Vtg) and back-gate (Vbg) voltages. (e) The optical absorption spectrum of CO2 which is captured and reconstructed by the BP spectrometer. (f) Optical extinction spectra of a BP-based electro-optical modulator, indicating an up to 6% modulation depth with the gate bias from -150 to 150 V. Reprinted with permission from [163], copyright (2017) American Chemical Society. (g), (h) Waveguide-integrated MIR LEDs based on the BP functional layer. Reprinted with permission from [46], copyright (2020) American Chemical Society. (g) SEM image of BP LED integrated on a waveguide. The stacked van der Waals layers including BP functional layer, two graphite electrodes, and an hBN encapsulation layer. (h) The spatially resolved electroluminescence mapping image of the LED, where the white dash lines draw two electrodes and the dark dash line draws the silicon waveguide.
Figure 11. Interface and surface engineering of BP for photonic applications. (a) Electro-spun BP-PVP membrane for ultrafast pulse generations. Reproduced with permission from [48], John Wiley & Sons. [© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim]. (b)-(d) Ink-printed BP as saturable absorbers for mode-locked fiber lasers. Reproduced from [50]. CC BY 4.0. (b) Schematic illustration that shows two fiber end-facets sandwich the ink-printed BP membrane for fiber integration. (c) Autocorrelation trace of the obtained mode-locking pulses. (d) Wavelength spectra of long-term stable operation across 30 d. (e), (f) Four-wave mixing devices based on BP-deposited nonlinear fibers for all-optical modulation. Reproduced from [52]. CC BY 4.0. (e) Optical spectra of the generated signals by the four-wave mixing effects with the modulation frequency from 0.13 to 20 GHz. (f) Optical spectra of the signals evolving by tuning the channel distance from 0.1 to 1.3 nm. (g), (h) Ultrafast optical switch based on interface polaritons in the SiO2/BP/SiO2 heterostructure. Reprinted from [51] by permission from Springer Nature Customer Service Centre GmbH. (g) Schematic diagram of the setup and the device where two SiO2 layers sandwich BP. (h) Scattered near-field intensity images in which the excitation and decay process of a hybrid phonon-plasmon-polariton mode are observed within a ten ps time scale.
Table 1. Passivation techniques for improving air stability of BP. The monitored time only refers to the duration it is monitored using characterization techniques, which is not the maximum survival time of BP.
Passivation technique Type Monitored time Characterization method References ALD of AlOx overlayers Physical coating 14 days AFM and charge transport measurements [27] Al2O3/Teflon-AF encapsulation 4 months Charge transport measurements [147] PMMA coating 19 days Raman measurement [148] Organic monolayers PTCDA via vdW epitaxy Classical molecular dynamics (MD) simulations [149] hBN-BP-hBN sandwiched configuration 150 h Charge transport measurements [150] Noncovalent functionalization with 7,7,8,8-tetracyano-p-quinodimethane (TCNQ) Chemical functionalization 2 days Raman, AFM, FTIR, STEM-EELS [151] Noncovalent functionalization with 1-methyl-2-pyrrolidone (NMP) 8 days AFM, Raman, DFT calculations [152] Covalent functionalization with 4-nitrobenzene-diazonium (4-NBD) 10 days AFM, XPS, Raman, charge transport, DFT calculations [64] Covalent functionalization with Titanium sulfonate ligand (TiL4) 3 days NMR, Raman, XPS, AFM [65] Self-assembled octadecyltrichlorosilane (OTS) 28 days XPS. Raman, charge transport [144] O2 plasma etching + Al2O3 coating Combined passivation 2 months Phase-shifting interferometry, PL, Raman [146] O2 plasma etching + hBN covering + rapid thermal annealing 7 months STEM, PL, Raman [153] 
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