Monolayer group VI transition metal dichalcogenides(TMDs)have recently emerged as promising candidates for photonic and opto-valleytronic applications.The optoelectronic properties of these atomically-thin semiconduct...Monolayer group VI transition metal dichalcogenides(TMDs)have recently emerged as promising candidates for photonic and opto-valleytronic applications.The optoelectronic properties of these atomically-thin semiconducting crystals are strongly governed by the tightly bound electron-hole pairs such as excitons and trions(charged excitons).The anomalous spin and valley configurations at the conduction band edges in monolayer WS_(2)give rise to even more fascinating valley many-body complexes.Here we find that the indirect Q valley in the first Brillouin zone of monolayer WS_(2)plays a critical role in the formation of a new excitonic state,which has not been well studied.By employing a high-quality h-BN encapsulated WS_(2)field-effect transistor,we are able to switch the electron concentration within K-Q valleys at conduction band edges.Consequently,a distinct emission feature could be excited at the high electron doping region.Such feature has a competing population with the K valley trion,and experiences nonlinear power-law response and lifetime dynamics under doping.Our findings open up a new avenue for the study of valley many-body physics and quantum optics in semiconducting 2D materials,as well as provide a promising way of valley manipulation for next-generation entangled photonic devices.展开更多
Montmorillonites (MMT) was modified with nonionic surfactant Trion X-100 (OP-10) and anionic surfactants sodium stearate (SSTA) and sodium dodecyl benzene sulfonate (SDBS) respectively. In this study, the effects of a...Montmorillonites (MMT) was modified with nonionic surfactant Trion X-100 (OP-10) and anionic surfactants sodium stearate (SSTA) and sodium dodecyl benzene sulfonate (SDBS) respectively. In this study, the effects of anionic surfactant types and MMT types on modification montmorillonite were investigated. XRD analysis results showed that SSTA/OP-10/MMT and SDBS/OP-10/MMT were successfully obtained. The basal spacing of SSTA/OP-10/MMT reached 5.07nm and the SSTA intercalation reaction was relatively stable. Different types of MMT (Xinjiang natural sodium montmorillonite(MMT-1), Jianping sodium montmorillonite (MMT-2) and artificial sodium montmorillonite(MMT-3)) were modified with SSTA/OP-10. XRD test results showed that MMT-1, MMT-2 and MMT-3 can be modified by SSTA/OP-10. Anion-nonionic organic montmorillonite (SSTA/OP-10/MMT-1, SSTA/OP-10/MMT-2 and SSTA/OP-10/MMT-3 were successfully obtained respectively. The higher expansion capacity was found to be beneficial to organic modification.展开更多
Light-harvesters with long-lived excited states are desired for efficient solar energy conversion systems. Many solar-to-fuel conversion reactions, such as H2 evolution and CO2 reduction, require multiple sequential e...Light-harvesters with long-lived excited states are desired for efficient solar energy conversion systems. Many solar-to-fuel conversion reactions, such as H2 evolution and CO2 reduction, require multiple sequential electron transfer processes, which leads to a complicated situation that excited states involves not only excitons (electron-hole pairs) but also multi-excitons and charged excitons. While long-lived excitons can be obtained in various systems (e.g., semiconductor nanocrystals), multi-excitons and charged excitons are typically shorted-lived due to nonradiative Auger recombination pathways whereby the recombination energy of an exciton is quickly transferred to the third carrier on a few to hundreds of picoseconds timescale. In this work, we report a study of excitons, trions (an exciton plus an additional charge), and biexcitons in CdSe/CdTe colloidal quantum wells or nanoplatelets. The type- II band alignment effectively separates electrons and holes in space, leading to a single exciton lifetime of 340 ns which is -2 order of magnitudes longer than that in plane CdSe nanoplatelets. More importantly, the electron-hole separation also dramatically slows down Auger decay, giving rise to a trion lifetime of 70 ns and a biexciton lifetime of 11 ns, among the longest values ever reported for colloidal nanocrystals. The long-lived exciton, trion, and biexciton states, combined with the intrinsically strong light-absorption capability of two-dimensional systems, enable the CdSe/CdTe type-II nanoplatelets as promising light harvesters for efficient solar-to-fuel conversion reactions.展开更多
Two-dimensional(2D)2H-MoTe2 is a promising semiconductor because of its small bandgap,strong absorption,and low thermal conductivity.In this paper,we systematically study the optical and excitonic properties of atomic...Two-dimensional(2D)2H-MoTe2 is a promising semiconductor because of its small bandgap,strong absorption,and low thermal conductivity.In this paper,we systematically study the optical and excitonic properties of atomically thin 2H-MoTe2(1–5 layers).Due to the fact that the optical contrast and Raman spectra of 2H-MoTe2 with different thicknesses exhibit distinctly different behaviors,we establish a quantitative method by using optical images and Raman spectra to directly identify the layers of 2H-MoTe2 thin films.Besides,excitonic states and binding energy in monolayer/bilayer 2H-MoTe2 are measured by temperature-dependent photoluminescence(PL)spectroscopy.At temperature T=3.3 K,we can observe an exciton emission at^1.19 eV and trion emission at^1.16 eV for monolayer 2H-MoTe2.While at room temperature,the exciton emission and trion emission both disappear for their small binding energy.We determine the exciton binding energy to be 185 meV(179 meV),trion binding energy to be 20 meV(18 me V)for the monolayer(bilayer)2H-MoTe2.The thoroughly studies of the excitonic states in atomically thin 2H-MoTe2 will provide guidance for future practical applications.展开更多
In this paper, a negatively charged exciton trapped by a spherical parabolic quantum dot has been investigated. The energy spectra of low-lying states are calculated by means of matrix diagonalization. The important f...In this paper, a negatively charged exciton trapped by a spherical parabolic quantum dot has been investigated. The energy spectra of low-lying states are calculated by means of matrix diagonalization. The important feature of the low-lying states of the negatively charged excitons in a spherical quantum dot is obtained via an analysis of the energy spectra.展开更多
In recent years,two-dimensional(2D)materials have attracted extensive interests due to the large exciton binding energy different from bulk materials.Many peculiar properties have been discovered that have farreaching...In recent years,two-dimensional(2D)materials have attracted extensive interests due to the large exciton binding energy different from bulk materials.Many peculiar properties have been discovered that have farreaching perspectives in the next generation of optoelectronic devices.In this review,we introduce the forms of exciton existence in 2D materials and several promising 2D materials with good applications at first.Then,we summarize relevant contemporary tools for probing exciton dynamics and methods of regulating 2D exciton transport,for instance,electrical regulation,stress/surface wave regulation and moirépotential regulation,etc.Finally,we conclude the general development of regulation in 2D materials and propose several possible opportunities of application prospect.展开更多
In situ strain photoluminescence (PL) and Raman spectroscopy have been employed to exploit the evolutions of the electronic band structure and lattice vibrational responses of chemical vapor deposition (CVD)-grown...In situ strain photoluminescence (PL) and Raman spectroscopy have been employed to exploit the evolutions of the electronic band structure and lattice vibrational responses of chemical vapor deposition (CVD)-grown monolayer tungsten disulphide (WS2) under uniaxial tensile strain. Observable broadening and appearance of an extra small feature at the longer-wavelength side shoulder of the PL peak occur under 2.5% strain, which could indicate the direct-indirect bandgap transition and is further confirmed by our density-functional-theory calculations. As the strain increases further, the spectral weight of the indirect transition gradually increases. Over the entire strain range, with the increase of the strain, the light emissions corresponding to each optical transition, such as the direct bandgap transition (K-K) and indirect bandgap transition (F-K, ≥2.5%), exhibit a monotonous linear redshift. In addition, the binding energy of the indirect transition is found to be larger than that of the direct transition, and the slight lowering of the trion dissociation energy with increasing strain is observed. The strain was used to modulate not only the electronic band structure but also the lattice vibrations. The softening and splitting of the in-plane E' mode is observed under uniaxial tensile strain, and polarization-dependent Raman spectroscopy confirms the observed zigzag-oriented edge of WS2 grown by CVD in previous studies. These findings enrich our understanding of the strained states of monolayer transition-metal dichalcogenide (TMD) materials and lay a foundation for developing applications exploiting their strain-dependent optical properties, including the strain detection and light-emission modulation of such emerging two-dimensional TMDs.展开更多
Monolayer transition metal dichalcogenides have emerged as promising mat erials for opt oelectTonic and nanophotonic devices.However,the low photoluminescence(PL)quantum yield(QY)hinders their various potential applic...Monolayer transition metal dichalcogenides have emerged as promising mat erials for opt oelectTonic and nanophotonic devices.However,the low photoluminescence(PL)quantum yield(QY)hinders their various potential applications.Here we engineer and enhance the PL intensity of monolayer WS_(2)by femtosecond laser irradiation.More than two orders of magnitude enhancement of PL intensity as compared to the as-prepared sample is determined.Furthermore,the engineering time is shortened by three orders of magnitude as compared to the improvement of PL intensity by continuous-wave laser irradiation.Based on the evolution of PL spectra,we attribute the giant PL enhancement to the conversion from trion emission to exciton,as well as the improvement of the QY when exciton and trion are localized to the new-formed defects.We have created microstructures on the monolayer WS_(2)based on the enhancement of PL intensity,where the engineered structures can be stably stored for more than three years.This flexible approach with the feature of excellent long-term storage stability is promising for applications in information storage,display technology,and opto electronic devices.展开更多
Mixed dimensional van der Waals(VdW)heterostructures constructed by one-dimensional(1D)and two-dimensional(2D)materials exhibit extra degree of freedom to modulate the electronic and optical properties due to the comb...Mixed dimensional van der Waals(VdW)heterostructures constructed by one-dimensional(1D)and two-dimensional(2D)materials exhibit extra degree of freedom to modulate the electronic and optical properties due to the combination of difterent dimensionalities.The charge transfer at the intertace between 1D and 2D materials plays a crucial role in the optoelectronic properties and performance of the heterostructure-based devices.Here,we stacked single-walled carbon nanotubes(SWNTs)on monolayer WS2 for a mixed dimensional vdW heterostructure,and investigated the local modulation of excitions and trions in WS2 by SWNTs.Different directions of charge transfer between SWNTs and WSz are evidenced by the photoluminescence(PL)spectra of WS2.The PL intensity can be either enhanced or weakened by individual SWNTs.In our work,the PL intensity of WS2 is enhanced and the exciton peak position heterostructure is red-shifted about 3 meV due to the charge transfer from WS2 to an individual SWNT(SWNT#1).The change of PL by another SWNT(SWNT#2)can not be well-resolved in far fild,but scanning near field optical microscope(SNOM)measurements show that the PL intensity of WS2 is weakened by the SWNT.The peak position of exciton is blue-shifted by^1 meV while that of trion is redshifted by^1 meV due to the charge transfer from the SWNT to WS2,These results give insight into the charge transfer at the interface of SWNTWS2 heterostructure,and can be useful for design of optoelectronic devices based on mixed dimensional vdW heterostructures.展开更多
Strain-engineered silicon nanocrystals(SiNCs)have recently been shown to possess direct bandgap.Here,we report the observation of a rich structure in the single-nanocrystal photoluminescence spectra of strain-engineer...Strain-engineered silicon nanocrystals(SiNCs)have recently been shown to possess direct bandgap.Here,we report the observation of a rich structure in the single-nanocrystal photoluminescence spectra of strain-engineered direct-bandgap SiNCs in the temperature range of 9–300 K.The relationship between individual types of spectra is discussed,and the numerical modeling of spectral diffusion of the experimentally acquired spectra reveals a common origin for most types.The intrinsic spectral shape is shown to be a structure that contains three peaks,approximately 150 meV apart,each of which possesses a Si phonon substructure.Narrow spectral lines,reaching ≤ meV at 20 K,are detected.The observed temperature dependence of the spectral structure can be assigned to the radiative recombination of positively charged trions,in contrast to several previous reports linking a very similar shape to phonons in the surface capping layers.Our result serves as strong additional support for the direct-bandgap nature of the investigated SiNCs.展开更多
基金the strong support from Singapore Ministry of Education via AcRF Tier 3 Programme “Geometrical Quantum Materials” (MOE2018-T3-1-002)AcRF Tier 2 grants (MOE2017-T2-1040)+7 种基金the National Natural Science Foundation of China (Grant No. 61435010)the National Natural Science Foundation of China (Grant No. 61905156)the National Natural Science Foundation of China (Grant No. 61575010)the China Postdoctoral Science Foundation (Grant No. 2017M622764)the Natural Science Foundation of Fujian Province (Grant No. 2022J01555)the Beijing Municipal Natural Science Foundation (Grant No. 4162016)the financial support of the Presidential Postdoctoral Fellowship program of the Nanyang Technological Universitysupport from the Elemental Strategy Initiative conducted by the MEXT, Japan and the CREST (JPMJCR15F3), JST
文摘Monolayer group VI transition metal dichalcogenides(TMDs)have recently emerged as promising candidates for photonic and opto-valleytronic applications.The optoelectronic properties of these atomically-thin semiconducting crystals are strongly governed by the tightly bound electron-hole pairs such as excitons and trions(charged excitons).The anomalous spin and valley configurations at the conduction band edges in monolayer WS_(2)give rise to even more fascinating valley many-body complexes.Here we find that the indirect Q valley in the first Brillouin zone of monolayer WS_(2)plays a critical role in the formation of a new excitonic state,which has not been well studied.By employing a high-quality h-BN encapsulated WS_(2)field-effect transistor,we are able to switch the electron concentration within K-Q valleys at conduction band edges.Consequently,a distinct emission feature could be excited at the high electron doping region.Such feature has a competing population with the K valley trion,and experiences nonlinear power-law response and lifetime dynamics under doping.Our findings open up a new avenue for the study of valley many-body physics and quantum optics in semiconducting 2D materials,as well as provide a promising way of valley manipulation for next-generation entangled photonic devices.
文摘Montmorillonites (MMT) was modified with nonionic surfactant Trion X-100 (OP-10) and anionic surfactants sodium stearate (SSTA) and sodium dodecyl benzene sulfonate (SDBS) respectively. In this study, the effects of anionic surfactant types and MMT types on modification montmorillonite were investigated. XRD analysis results showed that SSTA/OP-10/MMT and SDBS/OP-10/MMT were successfully obtained. The basal spacing of SSTA/OP-10/MMT reached 5.07nm and the SSTA intercalation reaction was relatively stable. Different types of MMT (Xinjiang natural sodium montmorillonite(MMT-1), Jianping sodium montmorillonite (MMT-2) and artificial sodium montmorillonite(MMT-3)) were modified with SSTA/OP-10. XRD test results showed that MMT-1, MMT-2 and MMT-3 can be modified by SSTA/OP-10. Anion-nonionic organic montmorillonite (SSTA/OP-10/MMT-1, SSTA/OP-10/MMT-2 and SSTA/OP-10/MMT-3 were successfully obtained respectively. The higher expansion capacity was found to be beneficial to organic modification.
文摘Light-harvesters with long-lived excited states are desired for efficient solar energy conversion systems. Many solar-to-fuel conversion reactions, such as H2 evolution and CO2 reduction, require multiple sequential electron transfer processes, which leads to a complicated situation that excited states involves not only excitons (electron-hole pairs) but also multi-excitons and charged excitons. While long-lived excitons can be obtained in various systems (e.g., semiconductor nanocrystals), multi-excitons and charged excitons are typically shorted-lived due to nonradiative Auger recombination pathways whereby the recombination energy of an exciton is quickly transferred to the third carrier on a few to hundreds of picoseconds timescale. In this work, we report a study of excitons, trions (an exciton plus an additional charge), and biexcitons in CdSe/CdTe colloidal quantum wells or nanoplatelets. The type- II band alignment effectively separates electrons and holes in space, leading to a single exciton lifetime of 340 ns which is -2 order of magnitudes longer than that in plane CdSe nanoplatelets. More importantly, the electron-hole separation also dramatically slows down Auger decay, giving rise to a trion lifetime of 70 ns and a biexciton lifetime of 11 ns, among the longest values ever reported for colloidal nanocrystals. The long-lived exciton, trion, and biexciton states, combined with the intrinsically strong light-absorption capability of two-dimensional systems, enable the CdSe/CdTe type-II nanoplatelets as promising light harvesters for efficient solar-to-fuel conversion reactions.
基金Project supported by the Natural Science Research Projects in Colleges and Universities of Jiangsu Province,China(Grant No.18KJD140003)
文摘Two-dimensional(2D)2H-MoTe2 is a promising semiconductor because of its small bandgap,strong absorption,and low thermal conductivity.In this paper,we systematically study the optical and excitonic properties of atomically thin 2H-MoTe2(1–5 layers).Due to the fact that the optical contrast and Raman spectra of 2H-MoTe2 with different thicknesses exhibit distinctly different behaviors,we establish a quantitative method by using optical images and Raman spectra to directly identify the layers of 2H-MoTe2 thin films.Besides,excitonic states and binding energy in monolayer/bilayer 2H-MoTe2 are measured by temperature-dependent photoluminescence(PL)spectroscopy.At temperature T=3.3 K,we can observe an exciton emission at^1.19 eV and trion emission at^1.16 eV for monolayer 2H-MoTe2.While at room temperature,the exciton emission and trion emission both disappear for their small binding energy.We determine the exciton binding energy to be 185 meV(179 meV),trion binding energy to be 20 meV(18 me V)for the monolayer(bilayer)2H-MoTe2.The thoroughly studies of the excitonic states in atomically thin 2H-MoTe2 will provide guidance for future practical applications.
基金The project supported by National Natural Science Foundation of China under Grant No. 10475021 and the Natured Science Foundation of Guangdong Province of China under Grant No. 04009519
文摘In this paper, a negatively charged exciton trapped by a spherical parabolic quantum dot has been investigated. The energy spectra of low-lying states are calculated by means of matrix diagonalization. The important feature of the low-lying states of the negatively charged excitons in a spherical quantum dot is obtained via an analysis of the energy spectra.
文摘In recent years,two-dimensional(2D)materials have attracted extensive interests due to the large exciton binding energy different from bulk materials.Many peculiar properties have been discovered that have farreaching perspectives in the next generation of optoelectronic devices.In this review,we introduce the forms of exciton existence in 2D materials and several promising 2D materials with good applications at first.Then,we summarize relevant contemporary tools for probing exciton dynamics and methods of regulating 2D exciton transport,for instance,electrical regulation,stress/surface wave regulation and moirépotential regulation,etc.Finally,we conclude the general development of regulation in 2D materials and propose several possible opportunities of application prospect.
基金This work is supported by the Singapore National Research Foundation NRF RF Award No. NRFRF2010- 07, MOE Tier 2 MOE2012-T2-2-049, A'Star SERC PSF grant No. 1321202101, and MOE Tier 1 MOE2013- T1-2-235. W. Huang acknowledges the support of the National Basic Research Program of China (973 Program) (No. 2015CB932200), the National Natural Science Foundation of China (NSFC) (Grant Nos. 21144004, 20974046, 21101095, 21003076, 20774043, 51173081, 50428303, 61136003, and 50428303), the Ministry of Education of China (No. IRT1148), the NSF of Jiangsu Province (Grant Nos. SBK201122680, 11KJB510017, BK2008053, 11KJB510017, BK2009025, 10KJB510013, and BZ2010043), and NUPT (Nos. NY210030 and NY211022). J. R Wang is grateful for the NSFC (No. 11474164), NSF of Jiangsu province (No. BK20131413), and the Jiangsu Specially-Appointed Professor program. Y. L. Wang thanks Luqing Wang, Dr. Xiaolong Zou, and Dr. Alex Kutana for the constructive discussion.
文摘In situ strain photoluminescence (PL) and Raman spectroscopy have been employed to exploit the evolutions of the electronic band structure and lattice vibrational responses of chemical vapor deposition (CVD)-grown monolayer tungsten disulphide (WS2) under uniaxial tensile strain. Observable broadening and appearance of an extra small feature at the longer-wavelength side shoulder of the PL peak occur under 2.5% strain, which could indicate the direct-indirect bandgap transition and is further confirmed by our density-functional-theory calculations. As the strain increases further, the spectral weight of the indirect transition gradually increases. Over the entire strain range, with the increase of the strain, the light emissions corresponding to each optical transition, such as the direct bandgap transition (K-K) and indirect bandgap transition (F-K, ≥2.5%), exhibit a monotonous linear redshift. In addition, the binding energy of the indirect transition is found to be larger than that of the direct transition, and the slight lowering of the trion dissociation energy with increasing strain is observed. The strain was used to modulate not only the electronic band structure but also the lattice vibrations. The softening and splitting of the in-plane E' mode is observed under uniaxial tensile strain, and polarization-dependent Raman spectroscopy confirms the observed zigzag-oriented edge of WS2 grown by CVD in previous studies. These findings enrich our understanding of the strained states of monolayer transition-metal dichalcogenide (TMD) materials and lay a foundation for developing applications exploiting their strain-dependent optical properties, including the strain detection and light-emission modulation of such emerging two-dimensional TMDs.
基金supported by the National Key Research and Development Program of China(Grant No.2017YFA0304203)the National Natural Science Foundation of China(Nos.91950109,61875109,61527824,61675119)+1 种基金the Natural Science Foundation of Shanxi Province(No.201901D111010(ZD)),PCSIRT(No.IRT_17R70),1331KSC,PTITPostgraduate Education Innovation Project of Shanxi Province(Nos.2019SY052,2020BY022).
文摘Monolayer transition metal dichalcogenides have emerged as promising mat erials for opt oelectTonic and nanophotonic devices.However,the low photoluminescence(PL)quantum yield(QY)hinders their various potential applications.Here we engineer and enhance the PL intensity of monolayer WS_(2)by femtosecond laser irradiation.More than two orders of magnitude enhancement of PL intensity as compared to the as-prepared sample is determined.Furthermore,the engineering time is shortened by three orders of magnitude as compared to the improvement of PL intensity by continuous-wave laser irradiation.Based on the evolution of PL spectra,we attribute the giant PL enhancement to the conversion from trion emission to exciton,as well as the improvement of the QY when exciton and trion are localized to the new-formed defects.We have created microstructures on the monolayer WS_(2)based on the enhancement of PL intensity,where the engineered structures can be stably stored for more than three years.This flexible approach with the feature of excellent long-term storage stability is promising for applications in information storage,display technology,and opto electronic devices.
基金the National Basic Research Program of China(Nos.2018YFA0703502 and 2016YFA0200104)the National Natural Science Foundation of China(Nos.51720105003,21790052,21573004 and 21974004).
文摘Mixed dimensional van der Waals(VdW)heterostructures constructed by one-dimensional(1D)and two-dimensional(2D)materials exhibit extra degree of freedom to modulate the electronic and optical properties due to the combination of difterent dimensionalities.The charge transfer at the intertace between 1D and 2D materials plays a crucial role in the optoelectronic properties and performance of the heterostructure-based devices.Here,we stacked single-walled carbon nanotubes(SWNTs)on monolayer WS2 for a mixed dimensional vdW heterostructure,and investigated the local modulation of excitions and trions in WS2 by SWNTs.Different directions of charge transfer between SWNTs and WSz are evidenced by the photoluminescence(PL)spectra of WS2.The PL intensity can be either enhanced or weakened by individual SWNTs.In our work,the PL intensity of WS2 is enhanced and the exciton peak position heterostructure is red-shifted about 3 meV due to the charge transfer from WS2 to an individual SWNT(SWNT#1).The change of PL by another SWNT(SWNT#2)can not be well-resolved in far fild,but scanning near field optical microscope(SNOM)measurements show that the PL intensity of WS2 is weakened by the SWNT.The peak position of exciton is blue-shifted by^1 meV while that of trion is redshifted by^1 meV due to the charge transfer from the SWNT to WS2,These results give insight into the charge transfer at the interface of SWNTWS2 heterostructure,and can be useful for design of optoelectronic devices based on mixed dimensional vdW heterostructures.
基金Czech Science Foundation Funding(Grant Nos.GPP204/12/P235(Katerina Kusova)and P108/12/G108(Ivan Pelant))and a L’Oreal-UNESCO for Women in Science scholarship(Katerina Kusova)are gratefully acknowledgedPart of this work was supported by the Czech-Japan collaborative project LG14246(Jan Valenta).
文摘Strain-engineered silicon nanocrystals(SiNCs)have recently been shown to possess direct bandgap.Here,we report the observation of a rich structure in the single-nanocrystal photoluminescence spectra of strain-engineered direct-bandgap SiNCs in the temperature range of 9–300 K.The relationship between individual types of spectra is discussed,and the numerical modeling of spectral diffusion of the experimentally acquired spectra reveals a common origin for most types.The intrinsic spectral shape is shown to be a structure that contains three peaks,approximately 150 meV apart,each of which possesses a Si phonon substructure.Narrow spectral lines,reaching ≤ meV at 20 K,are detected.The observed temperature dependence of the spectral structure can be assigned to the radiative recombination of positively charged trions,in contrast to several previous reports linking a very similar shape to phonons in the surface capping layers.Our result serves as strong additional support for the direct-bandgap nature of the investigated SiNCs.