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2D Materials
ACCEPTED MANUSCRIPT
Localized Emission from Laser-Irradiated Defects in Two-DimensionalHexagonal Boron NitrideTo cite this article before publication: SONGYAN HOU et al 2017 2D Mater. in press https://doi.org/10.1088/2053-1583/aa8e61
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Compared with large monolayers, the hBN monolayers domains intend to show narrower emissions after
laser irradiation. Thus, we arise an assumption that the optical properties are closely related to size of hBN
and hBN flakes with smaller size of ~200 nm should exhibit better optical properties. To verify this, we
performed laser irradiation onto hBN monolayers and flakes with different laser powers. Figure 5 shows
optical properties of hBN monolayers and flakes after femtosecond laser processing. Bright fluorescence
was clearly observed at irradiated regions, indicating the formation of optically active defects or colour
centres. The defects in hBN monolayers have almost the same wavelength of emission with that in flakes,
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suggesting the same type of defects are induced by laser (Figure 5a and f). More importantly, we found
narrow emissions (1.4 nm width) in hBN flakes without damaging substrate after low laser power
processing. However, fluorescence was no longer observed from hBN monolayers after laser processing
without damaging substrate, suggesting the absence defects. This is due to hBN monolayers have a wide
bandgap (~6 eV) and the thickness (2.8 nm) is too low to absorb the energy of laser, resulting in most
energy of laser is transferred into substrate and no defect is created. At the same excitation, hBN flakes
have much stronger fluorescence than monolayers (Figure 5a, b, d, e and f), indicating that it is easier to
create colour centres in hBN flakes than monolayer.
Figure 5. Generation of localized colour centres in hBN monolayers. (a-c) and flakes(d-g). (a,b) PL imtensity mapping of laser irradiated regions in hBN monolayers. Inset: a typical PL spectrum taken from the blue circle in (a). (c) Corresponding microscope image of (a,b), and the implemented laser powers are: 1.25 W, 0.89 W,0.53 W,0.27 W and 0.10 W from right to left. (d,e,f) PL intensity mapping of laser irradiated regions in hBN flakes. Inset: a typical PL spectrum taken from the bright spot in (f). (g) Corresponding microscope image of (d,e,f), and the implemented laser powers are: 1.60 W,1.25 W, 0.89 W,0.53 W,0.27 W and 0.10 W from left to right. Scale bar: 10 μm.
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From Figure 5d, e and f, plenty of separate bright colourful spots were created after laser processing, of
which the majority are attributed to single defects hosted by hBN flakes. Figure 6 presents the lowest and
highest g2(0) among all measured single photon emitters in hBN flakes with corresponding PL images.
Each spot is measured at room temperature using a 40 μW excitation laser with an acquisition time of 20
s and were normalized (without background correction). The fitting reveals the values of g2(0) ranges from
0.20 to 0.42 among all single photon emitters in hBN flakes in Figure 5g. The fitted values of totτ in Figure
6a and b are 3.4 ns and 3.2 ns, respectively. Figure 6c and d show the diameter of bright spot is ~ 650 nm
which is the diffraction limitation of CCD camera, indicating true diffraction limited optical centre is
successfully induced. The bright spot in Figure 5f also demonstrates single photon emission with g2(0) =
0.25, indicating one single photon emitter can be determinstically engineered by laser processing without
damaging substrate.
Figure 6. Single photon emitters in hBN flakes. (a,b) Second order autocorrelation functions curves from individual colour centres in hBN flakes (red and blue open circles). Solid red and blue lines are fits using
equation. (c,d) PL images corresponding to (a) and (b). Scale bar: 1 μm.
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CONCLUSION
In conclusion, we successfully created colour centres in hBN monolayers and flakes via laser irradiation
and find the transformation from hBN to cBN at large hBN monolayers region. The strong and sharp
emission matches well with that of NBVN like point defects in hBN. Laser processed hBN flakes intends
to exhibit sharper emission, brighter colour centres and better single photon emissions compared with
monolayers. Our results offer a new approach to engineering defects in hBN and motivate more
endeavours to explore further the optical properties of 2D materials in the application of photonics and
quantum technology using laser irradiation.
ACKNOWLEDGMENTS
We thank to Jinjun Lin and EINST Technology, Singapore, for some experiments in Supplementary
Information. The authors acknowledge the Ministry of Education (MOE2016-T2-1-052 and MOE-RG-
170-15) and National Research Foundation of Singapore (NRF-CRP12-2013-04).
REFERENCES
[1] Geim A K and Grigorieva I V 2013 Van der Waals heterostructures Nature 499 419-25 [2] Butler S Z, Hollen S M, Cao L, Cui Y, Gupta J A, Gutiérrez H R, Heinz T F, Hong S S, Huang J and Ismach
A F 2013 Progress, challenges, and opportunities in two-dimensional materials beyond graphene ACS nano 7 2898-926
[3] Xia F, Wang H, Xiao D, Dubey M and Ramasubramaniam A 2014 Two-dimensional material nanophotonics Nature Photonics 8 899-907
[4] Rajendra D, Kawser A, Jia Woei W, Adam W, James Jian-Qiang L, Yaron D and Ishwara B B 2016 Anisotropic charge carrier transport in free-standing hexagonal boron nitride thin films Applied Physics Express 9 065801
[5] Matthew Y, Jiamin X and LeRoy B J 2014 Graphene on hexagonal boron nitride Journal of Physics: Condensed Matter 26 303201
[6] Wenjing Z, Qixing W, Yu C, Zhuo W and Andrew T S W 2016 Van der Waals stacked 2D layered materials for optoelectronics 2D Materials 3 022001
[7] Zhong L, Amber M, Natalie B, Shruti S, Kehao Z, Yifan S, Xufan L, Nicholas J B, Hongtao Y, Susan K F-S, Alexey C, Hui Z, Stephen M, Aaron M L, Kai X, Brian J L, Marija D, James C M H, Jiwoong P, Manish C, Raymond E S, Ali J, Mark C H, Joshua R and Mauricio T 2016 2D materials advances: from large scale synthesis and controlled heterostructures to improved characterization techniques, defects and applications 2D Materials 3 042001
[8] Watanabe K, Taniguchi T and Kanda H 2004 Direct-bandgap properties and evidence for ultraviolet lasing of hexagonal boron nitride single crystal Nat. Mater. 3 404-9
[9] Rubio A, Corkill J L and Cohen M L 1994 Theory of graphitic boron nitride nanotubes Physical Review B 49 5081
Page 15 of 18 AUTHOR SUBMITTED MANUSCRIPT - 2DM-101894.R1
123456789101112131415161718192021222324252627282930313233343536373839404142434445464748495051525354555657585960 A
ccep
ted
Man
uscr
ipt
[10] Yuanbo Z, Angel R and Guy Le L 2017 Emergent elemental two-dimensional materials beyond graphene Journal of Physics D: Applied Physics 50 053004
[11] Xu M, Liang T, Shi M and Chen H 2013 Graphene-like two-dimensional materials Chemical reviews 113 3766-98
[12] Dean C R, Young A F, Meric I, Lee C, Wang L, Sorgenfrei S, Watanabe K, Taniguchi T, Kim P and Shepard K 2010 Boron nitride substrates for high-quality graphene electronics Nat. Nanotechnol. 5 722-6
[13] Matos M J S, Mazzoni M S C and Chacham H 2014 Graphene–boron nitride superlattices: the role of point defects at the BN layer Nanotechnology 25 165705
[14] Dong Z, Dong-Bo Z, Fuhua Y, Hai-Qing L, Hongqi X and Kai C 2015 Interface engineering of electronic properties of graphene/boron nitride lateral heterostructures 2D Materials 2 041001
[15] Jin-Cheng Z, Liang Z, Kretinin A V, Morozov S V, Yi Bo W, Tun W, Xiaojun L, Fei R, Jingyu Z, Ching-Yu L, Jia-Cing C, Miao L, Hui-Qiong W, Geim A K and Novoselov K S 2016 High thermal conductivity of hexagonal boron nitride laminates 2D Materials 3 011004
[16] Lindsay L and Broido D 2011 Enhanced thermal conductivity and isotope effect in single-layer hexagonal boron nitride Physical Review B 84 155421
[17] Krivanek O L, Chisholm M F, Nicolosi V, Pennycook T J, Corbin G J, Dellby N, Murfitt M F, Own C S, Szilagyi Z S and Oxley M P 2010 Atom-by-atom structural and chemical analysis by annular dark-field electron microscopy Nature 464 571-4
[18] Simon Z, Péter M, Carlos A F V and Christian S 2016 Role of hexagonal boron nitride in protecting ferromagnetic nanostructures from oxidation 2D Materials 3 011008
[19] Watanabe K, Taniguchi T and Kanda H 2004 Ultraviolet luminescence spectra of boron nitride single crystals grown under high pressure and high temperature Physica status solidi (a) 201 2561-5
[20] Gao R, Yin L, Wang C, Qi Y, Lun N, Zhang L, Liu Y-X, Kang L and Wang X 2009 High-yield synthesis of boron nitride nanosheets with strong ultraviolet cathodoluminescence emission The Journal of Physical Chemistry C 113 15160-5
[21] Watanabe K, Taniguchi T, Niiyama T, Miya K and Taniguchi M 2009 Far-ultraviolet plane-emission handheld device based on hexagonal boron nitride Nature photonics 3 591-4
[22] Huang X, Tan C, Yin Z and Zhang H 2014 25th Anniversary Article: Hybrid Nanostructures Based on Two ‐Dimensional Nanomaterials Advanced Materials 26 2185-204
[23] Kubota Y, Watanabe K, Tsuda O and Taniguchi T 2007 Deep ultraviolet light-emitting hexagonal boron nitride synthesized at atmospheric pressure Science 317 932-4
[24] Tran T T, Bray K, Ford M J, Toth M and Aharonovich I 2016 Quantum emission from hexagonal boron nitride monolayers Nat. Nanotechnol. 11 37-41
[25] Tran T T, Elbadawi C, Totonjian D, Lobo C J, Grosso G, Moon H, Englund D R, Ford M J, Aharonovich I and Toth M 2016 Robust multicolor single photon emission from point defects in hexagonal boron nitride ACS nano 10 7331-8
[26] Machaka R, Erasmus R M and Derry T E 2010 Formation of cBN nanocrystals by He+ implantation into hBN Diamond and Related Materials 19 1131-4
[27] Guo Y, Qiu J and Guo W 2016 Mechanical and electronic coupling in few-layer graphene and hBN wrinkles: a first-principles study Nanotechnology 27 505702
[28] Attaccalite C, Bockstedte M, Marini A, Rubio A and Wirtz L 2011 Coupling of excitons and defect states in boron-nitride nanostructures Physical Review B 83 144115
[29] Orellana W and Chacham H 2001 Stability of native defects in hexagonal and cubic boron nitride Physical Review B 63 125205
[30] Kloke A, von Stetten F, Zengerle R and Kerzenmacher S 2011 Strategies for the fabrication of porous platinum electrodes Advanced Materials 23 4976-5008
[31] Dasgupta N P, Sun J, Liu C, Brittman S, Andrews S C, Lim J, Gao H, Yan R and Yang P 2014 25th anniversary article: semiconductor nanowires–synthesis, characterization, and applications Advanced materials 26 2137-84
[32] McClelland J, Scholten R, Palm E and Celotta R 1993 Laser-focused atomic deposition SCIENCE-NEW YORK THEN WASHINGTON- 262 877-
Page 16 of 18AUTHOR SUBMITTED MANUSCRIPT - 2DM-101894.R1
123456789101112131415161718192021222324252627282930313233343536373839404142434445464748495051525354555657585960 A
ccep
ted
Man
uscr
ipt
[33] Jersch J and Dickmann K 1996 Nanostructure fabrication using laser field enhancement in the near field of a scanning tunneling microscope tip Appl. Phys. Lett. 68 868-70
[34] Huang X, Yin Z, Wu S, Qi X, He Q, Zhang Q, Yan Q, Boey F and Zhang H 2011 Graphene ‐based materials: synthesis, characterization, properties, and applications Small 7 1876-902
[35] El-Kady M F, Strong V, Dubin S and Kaner R B 2012 Laser scribing of high-performance and flexible graphene-based electrochemical capacitors Science 335 1326-30
[36] Gattass R R and Mazur E 2008 Femtosecond laser micromachining in transparent materials Nature photonics 2 219-25
[37] Morales A M and Lieber C M 1998 A laser ablation method for the synthesis of crystalline semiconductor nanowires Science 279 208-11
[38] Dai Z R, Pan Z W and Wang Z L 2003 Novel nanostructures of functional oxides synthesized by thermal evaporation Adv. Funct. Mater. 13 9-24
[39] Buividas R, Aharonovich I, Seniutinas G, Wang X, Rapp L, Rode A, Taniguchi T and Juodkazis S 2015 Photoluminescence from voids created by femtosecond-laser pulses inside cubic-BN Opt. Lett. 40 5711-3
[40] Chen Y-C, Salter P S, Knauer S, Weng L, Frangeskou A C, Stephen C J, Ishmael S N, Dolan P R, Johnson S and Green B L 2016 Laser writing of coherent colour centres in diamond Nature Photonics
[41] Tay R Y, Griep M H, Mallick G, Tsang S H, Singh R S, Tumlin T, Teo E H T and Karna S P 2014 Growth of large single-crystalline two-dimensional boron nitride hexagons on electropolished copper Nano letters 14 839-46
[42] Wang Y, Zheng Y, Xu X, Dubuisson E, Bao Q, Lu J and Loh K P 2011 Electrochemical delamination of CVD-grown graphene film: toward the recyclable use of copper catalyst ACS nano 5 9927-33
[43] Birowosuto M D, Sumikura H, Matsuo S, Taniyama H, van Veldhoven P J, Nötzel R and Notomi M 2012 Fast Purcell-enhanced single photon source in 1,550-nm telecom band from a resonant quantum dot-cavity coupling Scientific reports 2
[44] Michler P, Imamoğlu A, Mason M, Carson P, Strouse G and Buratto S 2000 Quantum correlation among photons from a single quantum dot at room temperature Nature 406 968-70
[45] Castelletto S, Johnson B C, Zachreson C, Beke D, Balogh I, Ohshima T, Aharonovich I and Gali A 2014 Room temperature quantum emission from cubic silicon carbide nanoparticles ACS nano 8 7938-47
[46] Gholipour B, Adamo G, Cortecchia D, Krishnamoorthy H N S, Birowosuto M D, Zheludev N I and Soci C 2017 Organometallic Perovskite Metasurfaces Advanced Materials 29 1604268-n/a
[47] Levitas V I and Javanbakht M 2013 Phase field approach to interaction of phase transformation and dislocation evolution Appl. Phys. Lett. 102 251904
[48] Levitas V I, Ma Y, Hashemi J, Holtz M and Guven N 2006 Strain-induced disorder, phase transformations, and transformation-induced plasticity in hexagonal boron nitride under compression and shear in a rotational diamond anvil cell: In situ x-ray diffraction study and modeling The Journal of chemical physics 125 044507
[49] Liu A, Rong H, Jones R, Cohen O, Hak D and Paniccia M 2006 Optical amplification and lasing by stimulated Raman scattering in silicon waveguides J. Lightwave Technol. 24 1440-55
[50] Reich S, Ferrari A, Arenal R, Loiseau A, Bello I and Robertson J 2005 Resonant Raman scattering in cubic and hexagonal boron nitride Physical Review B 71 205201
[51] Reich S, Ferrari A C, Arenal R, Loiseau A, Bello I and Robertson J 2005 Resonant Raman scattering in cubic and hexagonal boron nitride Physical Review B 71 205201
[52] Werninghaus T, Hahn J, Richter F and Zahn D R T 1997 Raman spectroscopy investigation of size effects in cubic boron nitride Appl. Phys. Lett. 70 958-60
[53] Erasmus R and Comins J 2004 Photoluminescence spectroscopy of electron ‐irradiation induced fects in cubic boron nitride (cBN) physica status solidi (c) 1 2269-73
[54] Schuller J A, Karaveli S, Schiros T, He K, Yang S, Kymissis I, Shan J and Zia R 2013 Orientation of luminescent excitons in layered nanomaterials Nat. Nanotechnol. 8 271-6
[55] Shotan Z, Jayakumar H, Considine C R, Mackoit M e, Fedder H, Wrachtrup J r, Alkauskas A, Doherty M W, Menon V M and Meriles C A 2016 Photoinduced Modification of Single-Photon Emitters in Hexagonal Boron Nitride ACS Photonics
Page 17 of 18 AUTHOR SUBMITTED MANUSCRIPT - 2DM-101894.R1
123456789101112131415161718192021222324252627282930313233343536373839404142434445464748495051525354555657585960 A
ccep
ted
Man
uscr
ipt
[56] Neitzke O, Morfa A, Wolters J, Schell A W, Kewes G n and Benson O 2015 Investigation of line width narrowing and spectral jumps of single stable defect centers in ZnO at cryogenic temperature Nano letters 15 3024-9
[57] Fleury L, Segura J-M, Zumofen G, Hecht B and Wild U 2000 Nonclassical photon statistics in single-molecule fluorescence at room temperature Physical review letters 84 1148
Page 18 of 18AUTHOR SUBMITTED MANUSCRIPT - 2DM-101894.R1
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