Environmental Screening Effects in 2D Materials: Renormalization of the Bandgap, Electronic Structure, and Optical Spectra of Few-Layer Black Phosphorus

Qiu, Diana Y.; da Jornada, Felipe H.; Louie, Steven G.

doi:10.1021/acs.nanolett.7b01365

Environmental Screening Effects in 2D Materials: Renormalization of the Bandgap, Electronic Structure, and Optical Spectra of Few-Layer Black Phosphorus

Journal Article · Wed Jul 05 00:00:00 EDT 2017 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.7b01365· OSTI ID:1484732

^[1]; da Jornada, Felipe H. ^[1]; Louie, Steven G. ^[1]

Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Few-layer black phosphorus has recently emerged as a potential 2D semiconductor, notable for its widely tunable bandgap, highly anisotropic properties, and theoretically predicted large exciton binding energies. To avoid degradation, it has become common practice to encapsulate black phosphorus devices. It is generally assumed that this encapsulation does not qualitatively affect their optical properties. In this work, we show that the contrary is true. We have performed ab initio GW and GW plus Bethe–Salpeter equation (GW-BSE) calculations to determine the quasiparticle (QP) band structure and optical spectrum of one-layer (1L) through four-layer (4L) black phosphorus, with and without encapsulation between hexagonal boron nitride and sapphire. We show that black phosphorus is exceptionally sensitive to environmental screening. Encapsulation reduces the exciton binding energy in 1L by as much as 70% and completely eliminates the presence of a bound exciton in the 4L structure. The reduction in the exciton binding energies is offset by a similarly large renormalization of the QP bandgap so that the optical gap remains nearly unchanged, yet the nature of the excited states and the qualitative features of the absorption spectrum change dramatically.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1484732

Journal Information:: Nano Letters, Journal Name: Nano Letters Journal Issue: 8 Vol. 17; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (46)

Semiempirical GGA-type density functional constructed with a long-range dispersion correction Grimme, Stefan Journal of Computational Chemistry, Vol. 27, Issue 15, p. 1787-1799 https://doi.org/10.1002/jcc.20495	journal	January 2006
Semiconductors — Basic Data Madelung, Otfried https://doi.org/10.1007/978-3-642-97675-9	book	January 1996
Electronic structure of black phosphorus: Tight binding approach Takao, Yukihiro; Morita, Akira Physica B+C, Vol. 105, Issue 1-3 https://doi.org/10.1016/0378-4363(81)90222-9	journal	May 1981
BerkeleyGW: A massively parallel computer package for the calculation of the quasiparticle and optical properties of materials and nanostructures Deslippe, Jack; Samsonidze, Georgy; Strubbe, David A. Computer Physics Communications, Vol. 183, Issue 6 https://doi.org/10.1016/j.cpc.2011.12.006	journal	June 2012
Probing the Role of Interlayer Coupling and Coulomb Interactions on Electronic Structure in Few-Layer MoSe ₂ Nanostructures Bradley, Aaron J.; M. Ugeda, Miguel; da Jornada, Felipe H. Nano Letters, Vol. 15, Issue 4 https://doi.org/10.1021/acs.nanolett.5b00160	journal	March 2015
Dielectric Genome of van der Waals Heterostructures Andersen, Kirsten; Latini, Simone; Thygesen, Kristian S. Nano Letters, Vol. 15, Issue 7 https://doi.org/10.1021/acs.nanolett.5b01251	journal	June 2015
Gate Switchable Transport and Optical Anisotropy in 90° Twisted Bilayer Black Phosphorus Cao, Ting; Li, Zhenglu; Qiu, Diana Y. Nano Letters, Vol. 16, Issue 9 https://doi.org/10.1021/acs.nanolett.6b02084	journal	August 2016
Probing the Influence of Dielectric Environment on Excitons in Monolayer WSe ₂ : Insight from High Magnetic Fields Stier, Andreas V.; Wilson, Nathan P.; Clark, Genevieve Nano Letters, Vol. 16, Issue 11 https://doi.org/10.1021/acs.nanolett.6b03276	journal	October 2016
Air-Stable Transport in Graphene-Contacted, Fully Encapsulated Ultrathin Black Phosphorus-Based Field-Effect Transistors Avsar, Ahmet; Vera-Marun, Ivan J.; Tan, Jun You ACS Nano, Vol. 9, Issue 4 https://doi.org/10.1021/acsnano.5b00289	journal	February 2015
Effective Passivation of Exfoliated Black Phosphorus Transistors against Ambient Degradation Wood, Joshua D.; Wells, Spencer A.; Jariwala, Deep Nano Letters, Vol. 14, Issue 12 https://doi.org/10.1021/nl5032293	journal	November 2014
Phosphorene: An Unexplored 2D Semiconductor with a High Hole Mobility Liu, Han; Neal, Adam T.; Zhu, Zhen ACS Nano, Vol. 8, Issue 4 https://doi.org/10.1021/nn501226z	journal	March 2014
Extraordinary Photoluminescence and Strong Temperature/Angle-Dependent Raman Responses in Few-Layer Phosphorene Zhang, Shuang; Yang, Jiong; Xu, Renjing ACS Nano, Vol. 8, Issue 9 https://doi.org/10.1021/nn503893j	journal	August 2014
Infrared fingerprints of few-layer black phosphorus Zhang, Guowei; Huang, Shenyang; Chaves, Andrey Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms14071	journal	January 2017
Rediscovering black phosphorus as an anisotropic layered material for optoelectronics and electronics Xia, Fengnian; Wang, Han; Jia, Yichen Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms5458	journal	July 2014
High-mobility transport anisotropy and linear dichroism in few-layer black phosphorus Qiao, Jingsi; Kong, Xianghua; Hu, Zhi-Xin Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms5475	journal	July 2014
Transport properties of pristine few-layer black phosphorus by van der Waals passivation in an inert atmosphere Doganov, Rostislav A.; O’Farrell, Eoin C. T.; Koenig, Steven P. Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms7647	journal	April 2015
High-quality sandwiched black phosphorus heterostructure and its quantum oscillations Chen, Xiaolong; Wu, Yingying; Wu, Zefei Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms8315	journal	June 2015
Giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor Ugeda, Miguel M.; Bradley, Aaron J.; Shi, Su-Fei Nature Materials, Vol. 13, Issue 12 https://doi.org/10.1038/nmat4061	journal	August 2014
Photooxidation and quantum confinement effects in exfoliated black phosphorus Favron, Alexandre; Gaufrès, Etienne; Fossard, Frédéric Nature Materials, Vol. 14, Issue 8 https://doi.org/10.1038/nmat4299	journal	May 2015
Black phosphorus field-effect transistors Li, Likai; Yu, Yijun; Ye, Guo Jun Nature Nanotechnology, Vol. 9, Issue 5 https://doi.org/10.1038/nnano.2014.35	journal	March 2014
Highly anisotropic and robust excitons in monolayer black phosphorus Wang, Xiaomu; Jones, Aaron M.; Seyler, Kyle L. Nature Nanotechnology, Vol. 10, Issue 6 https://doi.org/10.1038/nnano.2015.71	journal	April 2015
Direct observation of the layer-dependent electronic structure in phosphorene Li, Likai; Kim, Jonghwan; Jin, Chenhao Nature Nanotechnology, Vol. 12, Issue 1 https://doi.org/10.1038/nnano.2016.171	journal	September 2016
Optical constants of sapphire (α‐Al ₂ O ₃ ) single crystals Harman, Alang Kasim; Ninomiya, Susumu; Adachi, Sadao Journal of Applied Physics, Vol. 76, Issue 12 https://doi.org/10.1063/1.357922	journal	December 1994
Electric field effect in ultrathin black phosphorus Koenig, Steven P.; Doganov, Rostislav A.; Schmidt, Hennrik Applied Physics Letters, Vol. 104, Issue 10 https://doi.org/10.1063/1.4868132	journal	March 2014
QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502 https://doi.org/10.1088/0953-8984/21/39/395502	journal	September 2009
Isolation and characterization of few-layer black phosphorus Castellanos-Gomez, Andres; Vicarelli, Leonardo; Prada, Elsa 2D Materials, Vol. 1, Issue 2 https://doi.org/10.1088/2053-1583/1/2/025001	journal	June 2014
Gate tunable quantum oscillations in air-stable and high mobility few-layer phosphorene heterostructures Gillgren, Nathaniel; Wickramaratne, Darshana; Shi, Yanmeng 2D Materials, Vol. 2, Issue 1 https://doi.org/10.1088/2053-1583/2/1/011001	journal	December 2014
Environmental instability of few-layer black phosphorus Island, Joshua O.; Steele, Gary A.; Zant, Herre S. J. van der 2D Materials, Vol. 2, Issue 1 https://doi.org/10.1088/2053-1583/2/1/011002	journal	January 2015
Quasiparticle energies, excitons, and optical spectra of few-layer black phosphorus Tran, Vy; Fei, Ruixiang; Yang, Li 2D Materials, Vol. 2, Issue 4 https://doi.org/10.1088/2053-1583/2/4/044014	journal	November 2015
Lattice Infrared Spectra of Boron Nitride and Boron Monophosphide Gielisse, P. J.; Mitra, S. S.; Plendl, J. N. Physical Review, Vol. 155, Issue 3 https://doi.org/10.1103/PhysRev.155.1039	journal	March 1967
Electron correlation in semiconductors and insulators: Band gaps and quasiparticle energies Hybertsen, Mark S.; Louie, Steven G. Physical Review B, Vol. 34, Issue 8, p. 5390-5413 https://doi.org/10.1103/PhysRevB.34.5390	journal	October 1986
Electron-hole excitations and optical spectra from first principles Rohlfing, Michael; Louie, Steven G. Physical Review B, Vol. 62, Issue 8 https://doi.org/10.1103/PhysRevB.62.4927	journal	August 2000
Quasiparticle band structure calculation of monolayer, bilayer, and bulk MoS 2 Cheiwchanchamnangij, Tawinan; Lambrecht, Walter R. L. Physical Review B, Vol. 85, Issue 20 https://doi.org/10.1103/PhysRevB.85.205302	journal	May 2012
Layer-controlled band gap and anisotropic excitons in few-layer black phosphorus Tran, Vy; Soklaski, Ryan; Liang, Yufeng Physical Review B, Vol. 89, Issue 23 https://doi.org/10.1103/PhysRevB.89.235319	journal	June 2014
Excitons in anisotropic two-dimensional semiconducting crystals Rodin, A. S.; Carvalho, A.; Castro Neto, A. H. Physical Review B, Vol. 90, Issue 7 https://doi.org/10.1103/PhysRevB.90.075429	journal	August 2014
Tunable optical properties of multilayer black phosphorus thin films Low, Tony; Rodin, A. S.; Carvalho, A. Physical Review B, Vol. 90, Issue 7 https://doi.org/10.1103/PhysRevB.90.075434	journal	August 2014
Anisotropic exciton Stark shift in black phosphorus Chaves, A.; Low, Tony; Avouris, P. Physical Review B, Vol. 91, Issue 15 https://doi.org/10.1103/PhysRevB.91.155311	journal	April 2015
Excitons in van der Waals heterostructures: The important role of dielectric screening Latini, S.; Olsen, T.; Thygesen, K. S. Physical Review B, Vol. 92, Issue 24 https://doi.org/10.1103/PhysRevB.92.245123	journal	December 2015
Screening and many-body effects in two-dimensional crystals: Monolayer MoS 2 Qiu, Diana Y.; da Jornada, Felipe H.; Louie, Steven G. Physical Review B, Vol. 93, Issue 23 https://doi.org/10.1103/PhysRevB.93.235435	journal	June 2016
Strain-controlled fundamental gap and structure of bulk black phosphorus Guan, Jie; Song, Wenshen; Yang, Li Physical Review B, Vol. 94, Issue 4 https://doi.org/10.1103/PhysRevB.94.045414	journal	July 2016
Nonuniform sampling schemes of the Brillouin zone for many-electron perturbation-theory calculations in reduced dimensionality da Jornada, Felipe H.; Qiu, Diana Y.; Louie, Steven G. Physical Review B, Vol. 95, Issue 3 https://doi.org/10.1103/PhysRevB.95.035109	journal	January 2017
Optical Spectrum of MoS 2 : Many-Body Effects and Diversity of Exciton States Qiu, Diana Y.; da Jornada, Felipe H.; Louie, Steven G. Physical Review Letters, Vol. 111, Issue 21 https://doi.org/10.1103/PhysRevLett.111.216805	journal	November 2013
Strain-Induced Gap Modification in Black Phosphorus Rodin, A. S.; Carvalho, A.; Castro Neto, A. H. Physical Review Letters, Vol. 112, Issue 17 https://doi.org/10.1103/PhysRevLett.112.176801	journal	May 2014
Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer WS 2 Chernikov, Alexey; Berkelbach, Timothy C.; Hill, Heather M. Physical Review Letters, Vol. 113, Issue 7 https://doi.org/10.1103/PhysRevLett.113.076802	journal	August 2014
Simple Screened Hydrogen Model of Excitons in Two-Dimensional Materials Olsen, Thomas; Latini, Simone; Rasmussen, Filip Physical Review Letters, Vol. 116, Issue 5 https://doi.org/10.1103/PhysRevLett.116.056401	journal	February 2016
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996

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