Quek Su Ying
Degree: PhD
Position: Associate Professor
Affiliation: NUS - Department of Physics
Research Type: Theory
Office: S16-06-16
Email: phyqsy@nus.edu.sg
Website: http://www.physics.nus.edu.sg/staff/queksy.html
Research Interests:
First principles calculations (mean field and many-electron perturbation theory)
Interface science
Emerging materials
Electronic energy level alignment and transport
CA2DM Publications:
2022 |
Noori, Keian; Xuan, Fengyuan; Quek, Su Ying Origin of contact polarity at metal-2D transition metal dichalcogenide interfaces Journal Article NPJ 2D MATERIALS AND APPLICATIONS, 6 (1), 2022. @article{ISI:000876057300001, title = {Origin of contact polarity at metal-2D transition metal dichalcogenide interfaces}, author = {Keian Noori and Fengyuan Xuan and Su Ying Quek}, doi = {10.1038/s41699-022-00349-x}, times_cited = {0}, year = {2022}, date = {2022-10-14}, journal = {NPJ 2D MATERIALS AND APPLICATIONS}, volume = {6}, number = {1}, publisher = {NATURE PORTFOLIO}, address = {HEIDELBERGER PLATZ 3, BERLIN, 14197, GERMANY}, abstract = {Using state-of-the-art ab initio GW many-body perturbation theory calculations, we show that monolayer MoS2 on Au is a p-type contact, in contrast to the vast majority of theoretical predictions using density functional theory. The predominantly n-type behaviour observed experimentally for MoS2/Au junctions can be attributed to the presence of sulfur vacancies, which pin the Fermi level. GW calculations on WSe2/Au junctions likewise predict p-type contacts for pristine WSe2 and n-type contacts for junctions with selenium vacancies. Experimentally, WSe2/metal junctions are predominantly p-type or ambipolar, with p-type junctions being observed for selenium-deficient WSe2, suggesting that selenium vacancies are not effective in pinning the Fermi level for WSe2/metal junctions. We rationalize these apparently contradictory results by noting that selenium vacancies in WSe2 are readily passivated by oxygen atoms. Taken together, our state-of-the-art calculations clearly elucidate the relation between contact polarity and atomic structure. We show that non-local exchange and correlation effects are critical for determining the energy level alignment and even the contact polarity (in the case of MoS2 on Au). We further reconcile a large body of experimental literature on TMDC/metal contact polarities by consideration of the defect chemistry.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Using state-of-the-art ab initio GW many-body perturbation theory calculations, we show that monolayer MoS2 on Au is a p-type contact, in contrast to the vast majority of theoretical predictions using density functional theory. The predominantly n-type behaviour observed experimentally for MoS2/Au junctions can be attributed to the presence of sulfur vacancies, which pin the Fermi level. GW calculations on WSe2/Au junctions likewise predict p-type contacts for pristine WSe2 and n-type contacts for junctions with selenium vacancies. Experimentally, WSe2/metal junctions are predominantly p-type or ambipolar, with p-type junctions being observed for selenium-deficient WSe2, suggesting that selenium vacancies are not effective in pinning the Fermi level for WSe2/metal junctions. We rationalize these apparently contradictory results by noting that selenium vacancies in WSe2 are readily passivated by oxygen atoms. Taken together, our state-of-the-art calculations clearly elucidate the relation between contact polarity and atomic structure. We show that non-local exchange and correlation effects are critical for determining the energy level alignment and even the contact polarity (in the case of MoS2 on Au). We further reconcile a large body of experimental literature on TMDC/metal contact polarities by consideration of the defect chemistry. |
Zhang, Zhepeng; Liang, Haidong; Loh, Leyi; Chen, Yifeng; Chen, Yuan; Watanabe, Kenji; Taniguchi, Takashi; Quek, Su Ying; Bosman, Michel; Bettiol, Andrew A; Eda, Goki Optically Active Chalcogen Vacancies in Monolayer Semiconductors Journal Article ADVANCED OPTICAL MATERIALS, 10 (23), 2022, ISSN: 2195-1071. @article{ISI:000852786000001, title = {Optically Active Chalcogen Vacancies in Monolayer Semiconductors}, author = {Zhepeng Zhang and Haidong Liang and Leyi Loh and Yifeng Chen and Yuan Chen and Kenji Watanabe and Takashi Taniguchi and Su Ying Quek and Michel Bosman and Andrew A Bettiol and Goki Eda}, doi = {10.1002/adom.202201350}, times_cited = {0}, issn = {2195-1071}, year = {2022}, date = {2022-09-12}, journal = {ADVANCED OPTICAL MATERIALS}, volume = {10}, number = {23}, publisher = {WILEY-V C H VERLAG GMBH}, address = {POSTFACH 101161, 69451 WEINHEIM, GERMANY}, abstract = {Defect engineering of atomically thin semiconducting crystals is an attractive route to developing single-photon sources and valleytronic devices. For these applications, defects with well-defined optical characteristics need to be generated in a precisely controlled manner. However, defect-induced optical features are often complicated by the presence of multiple defect species, hindering the identification of their structural origin. Here, we report systematic generation of optically active atomic defects in monolayer MoS2, WS2, MoSe2, and WSe2 via proton-beam irradiation. Defect-induced emissions are found to occur approximate to 100 to 200 meV below the neutral exciton peak, showing typical characteristics of localized excitons such as saturation at high-excitation rates and long lifetime. Using scanning transmission electron microscopy, it is shown that freshly created chalcogen vacancies are responsible for the localized exciton emission. Density functional theory and ab initio GW plus Bethe-Salpeter-equation calculations reveal that the observed emission can be attributed to transitions involving defect levels of chalcogen vacancy and the valence band edge state.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Defect engineering of atomically thin semiconducting crystals is an attractive route to developing single-photon sources and valleytronic devices. For these applications, defects with well-defined optical characteristics need to be generated in a precisely controlled manner. However, defect-induced optical features are often complicated by the presence of multiple defect species, hindering the identification of their structural origin. Here, we report systematic generation of optically active atomic defects in monolayer MoS2, WS2, MoSe2, and WSe2 via proton-beam irradiation. Defect-induced emissions are found to occur approximate to 100 to 200 meV below the neutral exciton peak, showing typical characteristics of localized excitons such as saturation at high-excitation rates and long lifetime. Using scanning transmission electron microscopy, it is shown that freshly created chalcogen vacancies are responsible for the localized exciton emission. Density functional theory and ab initio GW plus Bethe-Salpeter-equation calculations reveal that the observed emission can be attributed to transitions involving defect levels of chalcogen vacancy and the valence band edge state. |
Wang, Ziying; Wang, Zishen; Zhou, Xin; Fu, Wei; Li, Haohan; Liu, Chaofei; Qiao, Jingsi; Quek, Su Ying; Su, Chenliang; Feng, Yuanping; Loh, Kian Ping Giant g-factor in Self-Intercalated 2D TaS2 Journal Article SMALL, 18 (38), 2022, ISSN: 1613-6810. @article{ISI:000842350300001, title = {Giant \textit{g}-factor in Self-Intercalated 2D TaS_{2}}, author = {Ziying Wang and Zishen Wang and Xin Zhou and Wei Fu and Haohan Li and Chaofei Liu and Jingsi Qiao and Su Ying Quek and Chenliang Su and Yuanping Feng and Kian Ping Loh}, doi = {10.1002/smll.202201975}, times_cited = {0}, issn = {1613-6810}, year = {2022}, date = {2022-08-21}, journal = {SMALL}, volume = {18}, number = {38}, publisher = {WILEY-V C H VERLAG GMBH}, address = {POSTFACH 101161, 69451 WEINHEIM, GERMANY}, abstract = {Central to the application of spintronic devices is the ability to manipulate spins by electric and magnetic fields, which relies on a large Lande g-factor. The self-intercalation of layered transitional metal dichalcogenides with native metal atoms can serve as a new strategy to enhance the g-factor by inducing ferromagnetic instability in the system via interlayer charge transfer. Here, scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS) are performed to extract the g-factor and characterize the electronic structure of the self-intercalated phase of 2H-TaS2. In Ta7S12, a sharp density of states (DOS) peak due to the Ta intercalant appears at the Fermi level, which satisfies the Stoner criteria for spontaneous ferromagnetism, leading to spin split states. The DOS peak shows sensitivity to magnetic field up to 1.85 mV T-1, equivalent to an effective g-factor of approximate to 77. This work establishes self-intercalation as an approach for tuning the g-factor.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Central to the application of spintronic devices is the ability to manipulate spins by electric and magnetic fields, which relies on a large Lande g-factor. The self-intercalation of layered transitional metal dichalcogenides with native metal atoms can serve as a new strategy to enhance the g-factor by inducing ferromagnetic instability in the system via interlayer charge transfer. Here, scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS) are performed to extract the g-factor and characterize the electronic structure of the self-intercalated phase of 2H-TaS2. In Ta7S12, a sharp density of states (DOS) peak due to the Ta intercalant appears at the Fermi level, which satisfies the Stoner criteria for spontaneous ferromagnetism, leading to spin split states. The DOS peak shows sensitivity to magnetic field up to 1.85 mV T-1, equivalent to an effective g-factor of approximate to 77. This work establishes self-intercalation as an approach for tuning the g-factor. |
He, Wen; Wetherington, Maxwell T; Ulman, Kanchan Ajit; Robinson, Joshua A; Quek, Su Ying Interface-Mediated Resonant Raman Enhancement for Shear Modes in a 2D Polar Metal Journal Article JOURNAL OF PHYSICAL CHEMISTRY C, 126 (34), pp. 14581-14589, 2022, ISSN: 1932-7447. @article{ISI:000844406700001, title = {Interface-Mediated Resonant Raman Enhancement for Shear Modes in a 2D Polar Metal}, author = {Wen He and Maxwell T Wetherington and Kanchan Ajit Ulman and Joshua A Robinson and Su Ying Quek}, doi = {10.1021/acs.jpcc.2c04433}, times_cited = {0}, issn = {1932-7447}, year = {2022}, date = {2022-08-18}, journal = {JOURNAL OF PHYSICAL CHEMISTRY C}, volume = {126}, number = {34}, pages = {14581-14589}, publisher = {AMER CHEMICAL SOC}, address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA}, abstract = {2D polar metals synthesized by confinement heteroepitaxy at the SiC/graphene interface are covalently bound to the SiC substrate. In this work, we elucidate the importance of the SiC substrate, and specifically the Ga/Si interface, on the low frequency resonant Raman spectra of 2D Ga on SiC. The low-frequency Raman modes are dominated by in-plane shear modes in 2D Ga. We show that the frequency of these shear modes is modified by the presence of the substrate for few-layer Ga and that these shear modes couple strongly to the electronic states corresponding to the interface Ga and Si atoms. Consequently, resonant Raman enhancement occurs at laser incident energies that are resonant with the interband optical transitions involving these interface Ga and Si states. This resonant Raman enhancement is observed in laser-energy dependent measurements, an experimental signature of the strong electron-phonon coupling present in these 2D polar metals.}, keywords = {}, pubstate = {published}, tppubtype = {article} } 2D polar metals synthesized by confinement heteroepitaxy at the SiC/graphene interface are covalently bound to the SiC substrate. In this work, we elucidate the importance of the SiC substrate, and specifically the Ga/Si interface, on the low frequency resonant Raman spectra of 2D Ga on SiC. The low-frequency Raman modes are dominated by in-plane shear modes in 2D Ga. We show that the frequency of these shear modes is modified by the presence of the substrate for few-layer Ga and that these shear modes couple strongly to the electronic states corresponding to the interface Ga and Si atoms. Consequently, resonant Raman enhancement occurs at laser incident energies that are resonant with the interband optical transitions involving these interface Ga and Si states. This resonant Raman enhancement is observed in laser-energy dependent measurements, an experimental signature of the strong electron-phonon coupling present in these 2D polar metals. |
Abdelwahab, Ibrahim; Tilmann, Benjamin; Wu, Yaze; Giovanni, David; Verzhbitskiy, Ivan; Zhu, Menglong; Berte, Rodrigo; Xuan, Fengyuan; de Menezes, Leonardo S; Eda, Goki; Sum, Tze Chien; Quek, Su Ying; Maier, Stefan A; Loh, Kian Ping Giant second-harmonic generation in ferroelectric NbOI2 Journal Article NATURE PHOTONICS, 16 (9), pp. 644-+, 2022, ISSN: 1749-4885. @article{ISI:000819314600001, title = {Giant second-harmonic generation in ferroelectric NbOI_{2}}, author = {Ibrahim Abdelwahab and Benjamin Tilmann and Yaze Wu and David Giovanni and Ivan Verzhbitskiy and Menglong Zhu and Rodrigo Berte and Fengyuan Xuan and Leonardo S de Menezes and Goki Eda and Tze Chien Sum and Su Ying Quek and Stefan A Maier and Kian Ping Loh}, doi = {10.1038/s41566-022-01021-y}, times_cited = {0}, issn = {1749-4885}, year = {2022}, date = {2022-06-30}, journal = {NATURE PHOTONICS}, volume = {16}, number = {9}, pages = {644-+}, publisher = {NATURE PORTFOLIO}, address = {HEIDELBERGER PLATZ 3, BERLIN, 14197, GERMANY}, abstract = {Implementing nonlinear optical components in nanoscale photonic devices is challenged by phase-matching conditions requiring thicknesses in the order of hundreds of wavelengths, and is disadvantaged by the short optical interaction depth of nanometre-scale materials and weak photon-photon interactions. Here we report that ferroelectric NbOI2 nanosheets exhibit giant second-harmonic generation with conversion efficiencies that are orders of magnitude higher than commonly reported nonlinear crystals. The nonlinear response scales with layer thickness and is strain- and electrical-tunable; a record >0.2% absolute SHG conversion efficiency and an effective nonlinear susceptibility chi((2))(eff) in the order of 10(-9) m V-1 are demonstrated at an average pump intensity of 8 kW cm(-2). Due to the interplay between anisotropic polarization and excitonic resonance in NbOI2, the spatial profile of the polarized SHG response can be tuned by the excitation wavelength. Our results represent a new paradigm for ultrathin, efficient nonlinear optical components.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Implementing nonlinear optical components in nanoscale photonic devices is challenged by phase-matching conditions requiring thicknesses in the order of hundreds of wavelengths, and is disadvantaged by the short optical interaction depth of nanometre-scale materials and weak photon-photon interactions. Here we report that ferroelectric NbOI2 nanosheets exhibit giant second-harmonic generation with conversion efficiencies that are orders of magnitude higher than commonly reported nonlinear crystals. The nonlinear response scales with layer thickness and is strain- and electrical-tunable; a record >0.2% absolute SHG conversion efficiency and an effective nonlinear susceptibility chi((2))(eff) in the order of 10(-9) m V-1 are demonstrated at an average pump intensity of 8 kW cm(-2). Due to the interplay between anisotropic polarization and excitonic resonance in NbOI2, the spatial profile of the polarized SHG response can be tuned by the excitation wavelength. Our results represent a new paradigm for ultrathin, efficient nonlinear optical components. |
Reed-Lingenfelter, Serrae N; Chen, Yifeng; Yarali, Milad; Charboneau, David J; Curley, Julia B; Hynek, David J; Wang, Mengjing; Williams, Natalie L; Hazari, Nilay; Quek, Su Ying; Cha, Judy J Compact Super Electron-Donor to Monolayer MoS2 Journal Article NANO LETTERS, 22 (11), pp. 4501-4508, 2022, ISSN: 1530-6984. @article{ISI:000810028900001, title = {Compact Super Electron-Donor to Monolayer MoS_{2}}, author = {Serrae N Reed-Lingenfelter and Yifeng Chen and Milad Yarali and David J Charboneau and Julia B Curley and David J Hynek and Mengjing Wang and Natalie L Williams and Nilay Hazari and Su Ying Quek and Judy J Cha}, doi = {10.1021/acs.nanolett.2c01167}, times_cited = {0}, issn = {1530-6984}, year = {2022}, date = {2022-06-08}, journal = {NANO LETTERS}, volume = {22}, number = {11}, pages = {4501-4508}, publisher = {AMER CHEMICAL SOC}, address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA}, abstract = {The surface functionalization of two-dimensional (2D) materials with organic electron donors (OEDs) is a powerful tool to modulate the electronic properties of the material. Here we report a novel molecular dopant, Me-OED, that demonstrates record-breaking molecular doping to MoS2, achieving a carrier density of 1.10 +/- 0.37 X 10(14) cm(-2) at optimal functionalization conditions; the achieved carrier density is much higher than those by other OEDs such as benzyl viologen and an OED based on 4,4'-bipyridine. This impressive doping power is attributed to the compact size of Me-OED, which leads to high surface coverage on MoS2. To confirm, we study Bu-t-OED, which has an identical reduction potential to Me-OED but is significantly larger. Using field-effect transistor measurements and spectroscopic characterization, we estimate the doping powers of Me- and Bu-t-OED are 0.22-0.44 and 0.11 electrons per molecule, respectively, in good agreement with calculations. Our results demonstrate that the small size of Me-OED is critical to maximizing the surface coverage and molecular interactions with MoS2, enabling us to achieve unprecedented doping of MoS2.}, keywords = {}, pubstate = {published}, tppubtype = {article} } The surface functionalization of two-dimensional (2D) materials with organic electron donors (OEDs) is a powerful tool to modulate the electronic properties of the material. Here we report a novel molecular dopant, Me-OED, that demonstrates record-breaking molecular doping to MoS2, achieving a carrier density of 1.10 +/- 0.37 X 10(14) cm(-2) at optimal functionalization conditions; the achieved carrier density is much higher than those by other OEDs such as benzyl viologen and an OED based on 4,4'-bipyridine. This impressive doping power is attributed to the compact size of Me-OED, which leads to high surface coverage on MoS2. To confirm, we study Bu-t-OED, which has an identical reduction potential to Me-OED but is significantly larger. Using field-effect transistor measurements and spectroscopic characterization, we estimate the doping powers of Me- and Bu-t-OED are 0.22-0.44 and 0.11 electrons per molecule, respectively, in good agreement with calculations. Our results demonstrate that the small size of Me-OED is critical to maximizing the surface coverage and molecular interactions with MoS2, enabling us to achieve unprecedented doping of MoS2. |
He, Wen; Wetherington, Maxwell T; Ulman, Kanchan Ajit; Gray, Jennifer L; Robinson, Joshua A; Quek, Su Ying Shear Modes in a 2D Polar Metal Journal Article JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 13 (18), pp. 4015-4020, 2022, ISSN: 1948-7185. @article{ISI:000803568300007, title = {Shear Modes in a 2D Polar Metal}, author = {Wen He and Maxwell T Wetherington and Kanchan Ajit Ulman and Jennifer L Gray and Joshua A Robinson and Su Ying Quek}, doi = {10.1021/acs.jpclett.2c00719}, times_cited = {0}, issn = {1948-7185}, year = {2022}, date = {2022-05-12}, journal = {JOURNAL OF PHYSICAL CHEMISTRY LETTERS}, volume = {13}, number = {18}, pages = {4015-4020}, publisher = {AMER CHEMICAL SOC}, address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA}, abstract = {Low-frequency shear and breathing modes are important Raman signatures of two-dimensional (2D) materials, providing information on the number of layers and insights into interlayer interactions. We elucidate the nature of low-frequency modes in a 2D polar metal-2D Ga covalently bonded to a SiC substrate, using a first-principles Green's function-based approach. The low-frequency Raman modes are dominated by surface resonance modes, consisting primarily of out-of-phase shear modes in Ga, coupled to SiC phonons. Breathing modes are strongly coupled to the substrate and do not give rise to peaks in the phonon spectra. The highest-frequency shear mode blue-shifts significantly with increasing thickness, reflecting both an increase in the number of Ga layers and an increase in the effective interlayer force constant. The surface resonance modes evolve into localized 2D Ga modes as the phonon momentum increases. The predicted low-frequency modes are consistent with Raman measurements on 2D polar Ga.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Low-frequency shear and breathing modes are important Raman signatures of two-dimensional (2D) materials, providing information on the number of layers and insights into interlayer interactions. We elucidate the nature of low-frequency modes in a 2D polar metal-2D Ga covalently bonded to a SiC substrate, using a first-principles Green's function-based approach. The low-frequency Raman modes are dominated by surface resonance modes, consisting primarily of out-of-phase shear modes in Ga, coupled to SiC phonons. Breathing modes are strongly coupled to the substrate and do not give rise to peaks in the phonon spectra. The highest-frequency shear mode blue-shifts significantly with increasing thickness, reflecting both an increase in the number of Ga layers and an increase in the effective interlayer force constant. The surface resonance modes evolve into localized 2D Ga modes as the phonon momentum increases. The predicted low-frequency modes are consistent with Raman measurements on 2D polar Ga. |
Wu, Yaze; Abdelwahab, Ibrahim; Kwon, Ki Chang; Verzhbitskiy, Ivan; Wang, Lin; Liew, Weng Heng; Yao, Kui; Eda, Goki; Loh, Kian Ping; Shen, Lei; Quek, Su Ying Data-driven discovery of high performance layered van der Waals piezoelectric NbOI2 Journal Article NATURE COMMUNICATIONS, 13 (1), 2022. @article{ISI:000779784400014, title = {Data-driven discovery of high performance layered van der Waals piezoelectric NbOI_{2}}, author = {Yaze Wu and Ibrahim Abdelwahab and Ki Chang Kwon and Ivan Verzhbitskiy and Lin Wang and Weng Heng Liew and Kui Yao and Goki Eda and Kian Ping Loh and Lei Shen and Su Ying Quek}, doi = {10.1038/s41467-022-29495-y}, times_cited = {0}, year = {2022}, date = {2022-04-07}, journal = {NATURE COMMUNICATIONS}, volume = {13}, number = {1}, publisher = {NATURE PORTFOLIO}, address = {HEIDELBERGER PLATZ 3, BERLIN, 14197, GERMANY}, abstract = {The recent thrust toward flexible nanoscale devices creates a need for two-dimensional piezoelectric materials. Here, the authors find large piezoelectric response in NbOI2 flakes ranging from 4 nm to the bulk.}, keywords = {}, pubstate = {published}, tppubtype = {article} } The recent thrust toward flexible nanoscale devices creates a need for two-dimensional piezoelectric materials. Here, the authors find large piezoelectric response in NbOI2 flakes ranging from 4 nm to the bulk. |
Zhao, Xiaoxu; Qiao, Jingsi; Zhou, Xin; Chen, Hao; Tan, Jun You; Yu, Hongyi; Chan, Si Min; Li, Jing; Zhang, Henshui; Zhou, Jiadong; Dan, Jiadong; Liu, Zhen; Zhou, Wu; Liu, Zheng; Peng, Bo; Deng, Longjiang; Pennycook, Stephen John; Quek, Su Ying; Loh, Kian Ping Strong Moire Excitons in High-Angle Twisted Transition Metal Dichalcogenide Homobilayers with Robust Commensuration Journal Article NANO LETTERS , 22 (1), pp. 203-210, 2022, ISSN: 1530-6984. @article{ISI:000769996700029, title = {Strong Moire Excitons in High-Angle Twisted Transition Metal Dichalcogenide Homobilayers with Robust Commensuration }, author = {Xiaoxu Zhao and Jingsi Qiao and Xin Zhou and Hao Chen and Jun You Tan and Hongyi Yu and Si Min Chan and Jing Li and Henshui Zhang and Jiadong Zhou and Jiadong Dan and Zhen Liu and Wu Zhou and Zheng Liu and Bo Peng and Longjiang Deng and Stephen John Pennycook and Su Ying Quek and Kian Ping Loh}, doi = {10.1021/acs.nanolett.1c03622}, times_cited = {0}, issn = {1530-6984}, year = {2022}, date = {2022-01-12}, journal = {NANO LETTERS }, volume = {22}, number = {1}, pages = {203-210}, publisher = {AMER CHEMICAL SOC }, address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA }, abstract = {The burgeoning field of twistronics, which concerns how changing the relative twist angles between two materials creates new optoelectronic properties, offers a novel platform for studying twist-angle dependent excitonic physics. Herein, by surveying a range of hexagonal phase transition metal dichalcogenides (TMD) twisted homobilayers, we find that 21.8 +/- 1.0 degrees-twisted (root 7a x root 7a) and 27.8 +/- 1.0 degrees-twisted (root 13a x root 13a) bilayers account for nearly 20% of the total population of twisted bilayers in solution-phase restacked bilayers and can be found also in chemical vapor deposition (CVD) samples. Examining the optical properties associated with these twisted angles, we found that 21.8 +/- 1.0 degrees twisted MoS2 bilayers exhibit an intense moire exciton peak in the photoluminescence (PL) spectra, originating from the refolded Brillouin zones. Our work suggests that commensurately twisted TMD homobilayers with short commensurate wavelengths can have interesting optoelectronic properties that are different from the small twist angle counterparts. }, keywords = {}, pubstate = {published}, tppubtype = {article} } The burgeoning field of twistronics, which concerns how changing the relative twist angles between two materials creates new optoelectronic properties, offers a novel platform for studying twist-angle dependent excitonic physics. Herein, by surveying a range of hexagonal phase transition metal dichalcogenides (TMD) twisted homobilayers, we find that 21.8 +/- 1.0 degrees-twisted (root 7a x root 7a) and 27.8 +/- 1.0 degrees-twisted (root 13a x root 13a) bilayers account for nearly 20% of the total population of twisted bilayers in solution-phase restacked bilayers and can be found also in chemical vapor deposition (CVD) samples. Examining the optical properties associated with these twisted angles, we found that 21.8 +/- 1.0 degrees twisted MoS2 bilayers exhibit an intense moire exciton peak in the photoluminescence (PL) spectra, originating from the refolded Brillouin zones. Our work suggests that commensurately twisted TMD homobilayers with short commensurate wavelengths can have interesting optoelectronic properties that are different from the small twist angle counterparts. |
2021 |
Zhao, Xiaoxu; Qiao, Jingsi; Zhou, Xin; Chen, Hao; Tan, Jun You; Yu, Hongyi; Chan, Si Min; Li, Jing; Zhang, Henshui; Zhou, Jiadong; Dan, Jiadong; Liu, Zhen; Zhou, Wu; Liu, Zheng; Peng, Bo; Deng, Longjiang; Pennycook, Stephen John; Quek, Su Ying; Loh, Kian Ping Strong Moire Excitons in High-Angle Twisted Transition Metal Dichalcogenide Homobilayers with Robust Commensuration Journal Article NANO LETTERS, 22 (1), pp. 203-210, 2021, ISSN: 1530-6984. @article{ISI:000734459700001, title = {Strong Moire Excitons in High-Angle Twisted Transition Metal Dichalcogenide Homobilayers with Robust Commensuration}, author = {Xiaoxu Zhao and Jingsi Qiao and Xin Zhou and Hao Chen and Jun You Tan and Hongyi Yu and Si Min Chan and Jing Li and Henshui Zhang and Jiadong Zhou and Jiadong Dan and Zhen Liu and Wu Zhou and Zheng Liu and Bo Peng and Longjiang Deng and Stephen John Pennycook and Su Ying Quek and Kian Ping Loh}, doi = {10.1021/acs.nanolett.1c03622}, times_cited = {0}, issn = {1530-6984}, year = {2021}, date = {2021-12-20}, journal = {NANO LETTERS}, volume = {22}, number = {1}, pages = {203-210}, publisher = {AMER CHEMICAL SOC}, address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA}, abstract = {The burgeoning field of twistronics, which concerns how changing the relative twist angles between two materials creates new optoelectronic properties, offers a novel platform for studying twist-angle dependent excitonic physics. Herein, by surveying a range of hexagonal phase transition metal dichalcogenides (TMD) twisted homobilayers, we find that 21.8 +/- 1.0 degrees-twisted (root 7a x root 7a) and 27.8 +/- 1.0 degrees-twisted (root 13a x root 13a) bilayers account for nearly 20% of the total population of twisted bilayers in solution-phase restacked bilayers and can be found also in chemical vapor deposition (CVD) samples. Examining the optical properties associated with these twisted angles, we found that 21.8 +/- 1.0 degrees twisted MoS2 bilayers exhibit an intense moire exciton peak in the photoluminescence (PL) spectra, originating from the refolded Brillouin zones. Our work suggests that commensurately twisted TMD homobilayers with short commensurate wavelengths can have interesting optoelectronic properties that are different from the small twist angle counterparts.}, keywords = {}, pubstate = {published}, tppubtype = {article} } The burgeoning field of twistronics, which concerns how changing the relative twist angles between two materials creates new optoelectronic properties, offers a novel platform for studying twist-angle dependent excitonic physics. Herein, by surveying a range of hexagonal phase transition metal dichalcogenides (TMD) twisted homobilayers, we find that 21.8 +/- 1.0 degrees-twisted (root 7a x root 7a) and 27.8 +/- 1.0 degrees-twisted (root 13a x root 13a) bilayers account for nearly 20% of the total population of twisted bilayers in solution-phase restacked bilayers and can be found also in chemical vapor deposition (CVD) samples. Examining the optical properties associated with these twisted angles, we found that 21.8 +/- 1.0 degrees twisted MoS2 bilayers exhibit an intense moire exciton peak in the photoluminescence (PL) spectra, originating from the refolded Brillouin zones. Our work suggests that commensurately twisted TMD homobilayers with short commensurate wavelengths can have interesting optoelectronic properties that are different from the small twist angle counterparts. |
Xuan, Fengyuan; Quek, Su Ying Valley-filling instability and critical magnetic field for interaction-enhanced Zeeman response in doped WSe2 monolayers Journal Article NPJ COMPUTATIONAL MATERIALS, 7 (1), 2021. @article{ISI:000728571700001, title = {Valley-filling instability and critical magnetic field for interaction-enhanced Zeeman response in doped WSe_{2} monolayers}, author = {Fengyuan Xuan and Su Ying Quek}, doi = {10.1038/s41524-021-00665-8}, times_cited = {8}, year = {2021}, date = {2021-12-09}, journal = {NPJ COMPUTATIONAL MATERIALS}, volume = {7}, number = {1}, publisher = {NATURE PORTFOLIO}, address = {HEIDELBERGER PLATZ 3, BERLIN, 14197, GERMANY}, abstract = {Carrier-doped transition metal dichalcogenide (TMD) monolayers are of great interest in valleytronics due to the large Zeeman response (g-factors) in these spin-valley-locked materials, arising from many-body interactions. We develop an ab initio approach based on many-body perturbation theory to compute the interaction-enhanced g-factors in carrier-doped materials. We show that the g-factors of doped WSe2 monolayers are enhanced by screened-exchange interactions resulting from magnetic-field-induced changes in band occupancies. Our interaction-enhanced g-factors g* agree well with experiment. Unlike traditional valleytronic materials such as silicon, the enhancement in g-factor vanishes beyond a critical magnetic field B-c achievable in standard laboratories. We identify ranges of g* for which this change in g-factor at B-c leads to a valley-filling instability and Landau level alignment, which is important for the study of quantum phase transitions in doped TMDs. We further demonstrate how to tune the g-factors and optimize the valley-polarization for the valley Hall effect.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Carrier-doped transition metal dichalcogenide (TMD) monolayers are of great interest in valleytronics due to the large Zeeman response (g-factors) in these spin-valley-locked materials, arising from many-body interactions. We develop an ab initio approach based on many-body perturbation theory to compute the interaction-enhanced g-factors in carrier-doped materials. We show that the g-factors of doped WSe2 monolayers are enhanced by screened-exchange interactions resulting from magnetic-field-induced changes in band occupancies. Our interaction-enhanced g-factors g* agree well with experiment. Unlike traditional valleytronic materials such as silicon, the enhancement in g-factor vanishes beyond a critical magnetic field B-c achievable in standard laboratories. We identify ranges of g* for which this change in g-factor at B-c leads to a valley-filling instability and Landau level alignment, which is important for the study of quantum phase transitions in doped TMDs. We further demonstrate how to tune the g-factors and optimize the valley-polarization for the valley Hall effect. |
Steves, Megan A; Rajabpour, Siavash; Wang, Ke; Dong, Chengye; He, Wen; Quek, Su Ying; Robinson, Joshua A; Knappenberger, Kenneth L Atomic-Level Structure Determines Electron-Phonon Scattering Rates in 2-D Polar Metal Heterostructures Journal Article ACS NANO, 15 (11), pp. 17780-17789, 2021, ISSN: 1936-0851. @article{ISI:000747115200058, title = {Atomic-Level Structure Determines Electron-Phonon Scattering Rates in 2-D Polar Metal Heterostructures}, author = {Megan A Steves and Siavash Rajabpour and Ke Wang and Chengye Dong and Wen He and Su Ying Quek and Joshua A Robinson and Kenneth L Knappenberger}, doi = {10.1021/acsnano.1c05944}, times_cited = {0}, issn = {1936-0851}, year = {2021}, date = {2021-11-23}, journal = {ACS NANO}, volume = {15}, number = {11}, pages = {17780-17789}, publisher = {AMER CHEMICAL SOC}, address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA}, abstract = {The electron dynamics of atomically thin 2-D polar metal heterostructures, which consisted of a few crystalline metal atomic layers intercalated between hexagonal silicon carbide and graphene grown from the silicon carbide, were studied using nearly degenerate transient absorption spectroscopy. Optical pumping created charge carriers in both the 2-D metals and graphene components. Wavelength-dependent probing suggests that graphene-to-metal carrier transfer occurred on a sub-picosecond time scale. Following rapid (<300 fs) carrier-carrier scattering, charge carriers monitored through the metal interband transition relaxed through several consecutive cooling mechanisms that included sub-picosecond carrier-phonon scattering and dissipation to the silicon carbide substrate over tens of picoseconds. By studying 2-D In, 2-D Ga, and a Ga/In alloy, we resolved accelerated electron-phonon scattering rates upon alloy formation as well as structural influences on the excitation of in-plane phonon shear modes. More rapid cooling in alloys is attributed to increased lattice disorder, which was observed through correlative polarization-resolved second harmonic generation and electron microscopy. This connection between the electronic relaxation rates, far-field optical responses, and metal lattice disorder is made possible by the intimate relation between nonlinear optical properties and atomic-level structure in these materials. These studies provided insights into electronic carrier dynamics in 2-D crystalline elemental metals, including resolving contributions from specific components of a 2-D metal-containing heterojunction. The correlative ultrafast spectroscopy and nonlinear microscopy results suggest that the energy dissipation rates can be tuned through atomic-level structures.}, keywords = {}, pubstate = {published}, tppubtype = {article} } The electron dynamics of atomically thin 2-D polar metal heterostructures, which consisted of a few crystalline metal atomic layers intercalated between hexagonal silicon carbide and graphene grown from the silicon carbide, were studied using nearly degenerate transient absorption spectroscopy. Optical pumping created charge carriers in both the 2-D metals and graphene components. Wavelength-dependent probing suggests that graphene-to-metal carrier transfer occurred on a sub-picosecond time scale. Following rapid (<300 fs) carrier-carrier scattering, charge carriers monitored through the metal interband transition relaxed through several consecutive cooling mechanisms that included sub-picosecond carrier-phonon scattering and dissipation to the silicon carbide substrate over tens of picoseconds. By studying 2-D In, 2-D Ga, and a Ga/In alloy, we resolved accelerated electron-phonon scattering rates upon alloy formation as well as structural influences on the excitation of in-plane phonon shear modes. More rapid cooling in alloys is attributed to increased lattice disorder, which was observed through correlative polarization-resolved second harmonic generation and electron microscopy. This connection between the electronic relaxation rates, far-field optical responses, and metal lattice disorder is made possible by the intimate relation between nonlinear optical properties and atomic-level structure in these materials. These studies provided insights into electronic carrier dynamics in 2-D crystalline elemental metals, including resolving contributions from specific components of a 2-D metal-containing heterojunction. The correlative ultrafast spectroscopy and nonlinear microscopy results suggest that the energy dissipation rates can be tuned through atomic-level structures. |
Ulman, Kanchan; Quek, Su Ying Organic-2D Material Heterostructures: A Promising Platform for Exciton Condensation and Multiplication Journal Article NANO LETTERS, 21 (20), pp. 8888-8894, 2021, ISSN: 1530-6984. @article{ISI:000713060900047, title = {Organic-2D Material Heterostructures: A Promising Platform for Exciton Condensation and Multiplication}, author = {Kanchan Ulman and Su Ying Quek}, doi = {10.1021/acs.nanolett.1c03435}, times_cited = {0}, issn = {1530-6984}, year = {2021}, date = {2021-10-18}, journal = {NANO LETTERS}, volume = {21}, number = {20}, pages = {8888-8894}, publisher = {AMER CHEMICAL SOC}, address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA}, abstract = {We predict that high temperature Bose-Einstein condensation of charge transfer excitons can be achieved in organic-two-dimensional (2D) material heterostructures, at similar to 50-100 K. Unlike 2D bilayers that can be angle-misaligned, organic-2D systems generally have momentum-direct low-energy excitons, thus favoring condensation. Our predictions are obtained for ZnPc-MoS2 using state-of-the-art first-principles calculations with the GW-BSE approach. The exciton energies we predict are in excellent agreement with recent experiments. The lowest energy charge transfer excitons in ZnPc-MoS2 are strongly bound with a spatial extent of similar to 1-2 nm and long lifetimes (tau(0) similar to 1 ns), making them ideal for exciton condensation. We also predict the emergence of inter-ZnPc excitons that are stabilized by the interaction of the molecules with the 2D substrate. This novel way of stabilizing intermolecular excitons by indirect substrate mediation suggests design strategies for singlet fission and exciton multiplication, which are important to overcome the Shockley-Queisser efficiency limit in solar cells.}, keywords = {}, pubstate = {published}, tppubtype = {article} } We predict that high temperature Bose-Einstein condensation of charge transfer excitons can be achieved in organic-two-dimensional (2D) material heterostructures, at similar to 50-100 K. Unlike 2D bilayers that can be angle-misaligned, organic-2D systems generally have momentum-direct low-energy excitons, thus favoring condensation. Our predictions are obtained for ZnPc-MoS2 using state-of-the-art first-principles calculations with the GW-BSE approach. The exciton energies we predict are in excellent agreement with recent experiments. The lowest energy charge transfer excitons in ZnPc-MoS2 are strongly bound with a spatial extent of similar to 1-2 nm and long lifetimes (tau(0) similar to 1 ns), making them ideal for exciton condensation. We also predict the emergence of inter-ZnPc excitons that are stabilized by the interaction of the molecules with the 2D substrate. This novel way of stabilizing intermolecular excitons by indirect substrate mediation suggests design strategies for singlet fission and exciton multiplication, which are important to overcome the Shockley-Queisser efficiency limit in solar cells. |
Chen, Yifeng; Quek, Su Ying Photophysical Characteristics of Boron Vacancy-Derived Defect Centers in Hexagonal Boron Nitride Journal Article JOURNAL OF PHYSICAL CHEMISTRY C, 125 (39), pp. 21791-21802, 2021, ISSN: 1932-7447. @article{ISI:000707043000051, title = {Photophysical Characteristics of Boron Vacancy-Derived Defect Centers in Hexagonal Boron Nitride}, author = {Yifeng Chen and Su Ying Quek}, doi = {10.1021/acs.jpcc.1c07729}, times_cited = {2}, issn = {1932-7447}, year = {2021}, date = {2021-09-23}, journal = {JOURNAL OF PHYSICAL CHEMISTRY C}, volume = {125}, number = {39}, pages = {21791-21802}, publisher = {AMER CHEMICAL SOC}, address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA}, abstract = {Single-photon emitter (SPE) sources are important building blocks for photonics-based quantum technologies. Recently, the highly bright and versatile SPEs from the two-dimensional insulator material hexagonal boron nitride (hBN) have attracted significant research interest. However, due to the variability of emitter species and properties, an exact correlation between the underlying atomistic structures and their photophysical properties is still lacking. In this work, we study six boron vacancy-derived defect centers in hBN (V-B(-), V-B + H, V-B2, VBCN, VBCN-, and VBCNCN) using advanced first-principles techniques, characterizing their quasiparticle defect levels, optical spectra and excitation energies, and magnetoresonance properties. These defects have been chosen because they are amenable to intentional creation under experimental conditions, such as electron or ion bombardment and carbon implantation. We establish the correlation between the underlying defect atomic structures and their photophysical properties, thus facilitating the identification of SPEs that have already been observed in experiments. Our results lead to clear insights into the very recent experiments where hBN SPEs were controlled intentionally. On the other hand, our results also serve as guidelines for the bottom-up design of defect emitter centers in hBN for target applications that require specific defect properties, such as emission in the telecom wavelength, optical addressability, and high radiative decay rates. This work thus provides a comprehensive understanding of the photophysical characteristics of V-B-derived defect-emitting centers, aiding in their identification and manipulation for tailored applications.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Single-photon emitter (SPE) sources are important building blocks for photonics-based quantum technologies. Recently, the highly bright and versatile SPEs from the two-dimensional insulator material hexagonal boron nitride (hBN) have attracted significant research interest. However, due to the variability of emitter species and properties, an exact correlation between the underlying atomistic structures and their photophysical properties is still lacking. In this work, we study six boron vacancy-derived defect centers in hBN (V-B(-), V-B + H, V-B2, VBCN, VBCN-, and VBCNCN) using advanced first-principles techniques, characterizing their quasiparticle defect levels, optical spectra and excitation energies, and magnetoresonance properties. These defects have been chosen because they are amenable to intentional creation under experimental conditions, such as electron or ion bombardment and carbon implantation. We establish the correlation between the underlying defect atomic structures and their photophysical properties, thus facilitating the identification of SPEs that have already been observed in experiments. Our results lead to clear insights into the very recent experiments where hBN SPEs were controlled intentionally. On the other hand, our results also serve as guidelines for the bottom-up design of defect emitter centers in hBN for target applications that require specific defect properties, such as emission in the telecom wavelength, optical addressability, and high radiative decay rates. This work thus provides a comprehensive understanding of the photophysical characteristics of V-B-derived defect-emitting centers, aiding in their identification and manipulation for tailored applications. |
Cheng, Nicholas Lin Quan; Xuan, Fengyuan; Spataru, Catalin D; Quek, Su Ying Charge Transfer Screening and Energy Level Alignment at Complex Organic-Inorganic Interfaces: A Tractable Ab Initio GW Approach Journal Article JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 12 (36), pp. 8841-8846, 2021, ISSN: 1948-7185. @article{ISI:000697334300019, title = {Charge Transfer Screening and Energy Level Alignment at Complex Organic-Inorganic Interfaces: A Tractable \textit{Ab Initio} GW Approach}, author = {Nicholas Lin Quan Cheng and Fengyuan Xuan and Catalin D Spataru and Su Ying Quek}, doi = {10.1021/acs.jpclett.1c02302}, times_cited = {1}, issn = {1948-7185}, year = {2021}, date = {2021-09-07}, journal = {JOURNAL OF PHYSICAL CHEMISTRY LETTERS}, volume = {12}, number = {36}, pages = {8841-8846}, publisher = {AMER CHEMICAL SOC}, address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA}, abstract = {Complex organic-inorganic interfaces are important for device and sensing applications. Charge transfer doping is prevalent in such applications and can affect the interfacial energy level alignments (ELA), which are determined by many-body interactions. We develop an approximate ab initio many-body GW approach that can capture many-body interactions due to interfacial charge transfer. The approach uses significantly less resources than a regular GW calculation but gives excellent agreement with benchmark GW calculations on an F4TCNQ/graphene interface. We find that many-body interactions due to charge transfer screening result in gate-tunable F4TCNQ HOMO-LUMO gaps. We further predict the ELA of a large system of experimental interest-4,4'-bis(dimethylamino)-bipyridine (DMAP-OED) on monolayer MoS2, where charge transfer screening results in an similar to 1 eV reduction of the molecular HOMO-LUMO gap. Comparison with a two-dimensional electron gas model reveals the importance of explicitly considering the intraband transitions in determining the charge transfer screening in organic-inorganic interface systems.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Complex organic-inorganic interfaces are important for device and sensing applications. Charge transfer doping is prevalent in such applications and can affect the interfacial energy level alignments (ELA), which are determined by many-body interactions. We develop an approximate ab initio many-body GW approach that can capture many-body interactions due to interfacial charge transfer. The approach uses significantly less resources than a regular GW calculation but gives excellent agreement with benchmark GW calculations on an F4TCNQ/graphene interface. We find that many-body interactions due to charge transfer screening result in gate-tunable F4TCNQ HOMO-LUMO gaps. We further predict the ELA of a large system of experimental interest-4,4'-bis(dimethylamino)-bipyridine (DMAP-OED) on monolayer MoS2, where charge transfer screening results in an similar to 1 eV reduction of the molecular HOMO-LUMO gap. Comparison with a two-dimensional electron gas model reveals the importance of explicitly considering the intraband transitions in determining the charge transfer screening in organic-inorganic interface systems. |