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Giant-Shell CdSe/CdS Nanocrystals: Exciton Coupling to Shell Phonons Investigated by Resonant Raman Spectroscopy
摘要： The interaction between excitons and phonons in semiconductor nanocrystals plays a crucial role in the exciton energy spectrum and dynamics, and thus in their optical properties. We investigate the exciton-phonon coupling in giant-shell CdSe/CdS core-shell nanocrystals via resonant Raman spectroscopy. The Huang-Rhys parameter is evaluated by the intensity ratio of the longitudinal-optical (LO) phonon of CdS with its first multiscattering (2LO) replica. We used four different excitation wavelengths in the range from the onset of the CdS shell absorption to well above the CdS shell band edge to get insight into resonance effects of the CdS LO phonon with high energy excitonic transitions. The isotropic spherical giant-shell nanocrystals show consistently stronger exciton-phonon coupling as compared to the anisotropic rod-shaped dot-in-rod (DiR) architecture, and the 2LO/LO intensity ratio decreases for excitation wavelengths approaching the CdS band edge. The strong exciton-phonon coupling in the spherical giant-shell nanocrystals can be related to the delocalization of the electronic wave functions. Furthermore, we observe the radial breathing modes of the GS nanocrystals and their overtones by ultra-low frequency Raman spectroscopy with nonresonant excitation, using laser energies well below the band gap of the heteronanocrystals, and highlight the differences between higher order optical and acoustic phonon modes.
关键词： Giant-shell nanocrystals,acoustic phonons,Dot-in-rods,Raman spectroscopy,Core-shell heterostructures,exciton-phonon coupling
更新于2025-09-23 15:23:52
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Fundamental Limit of the Emission Linewidths of Quantum Dots: An Ab Initio Study of CdSe Nanocrystals
摘要： The emission linewidth of a semiconducting nanocrystal (NC) significantly affects the performance in light-emitting applications but its fundamental limit is still elusive. Herein we analyze exciton-phonon coupling (EPC) from Huang-Rhys (HR) factors using ab initio calculations, and compute emission line shapes of CdSe NCs. When surface traps are absent, acoustic modes are found to dominate EPC. The computed linewidths are mainly determined by the size of NCs, being largely insensitive to the shape and crystal structure. Linewidths obtained in this work are much smaller than most measurements on the homogeneous linewidth, but they are consistent with a CdSe/CdxZn1?xSe (core/shell) NC [Park et al. Nat. Mater. 2019, 18, 249-255]. Based on this comparison, it is concluded that the large linewidths in most experiments originated from internal fields by surface (or interface) traps or quasi-type Ⅱ band alignment that amplify EPC. Thus, the present results on NCs with ideal passivation provide the fundamental minimum of homogeneous linewidths, indicating that only the CdSe/CdxZn1?xSe NC has achieved this limit through well-controlled synthesis of the shell structure. To further verify the role of internal fields, we model NCs with charged surface defects. We find that the internal field significantly increases HR factors and linewidths, in reasonable agreements with experiments on single cores. By revealing the fundamental limit of emission linewidths of quantum dots, this work will pave the way to engineering quantum dots with ultrasharp spectrum.
关键词： nanocrystals,photoluminescence,homogeneous linewidth,exciton-phonon coupling,surface traps,density functional theory,electroluminescence,quantum dots
更新于2025-09-19 17:13:59
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Spectroscopic monitoring of the evolution of size and structural defects in kinetic growth of CdSe quantum dots
摘要： We report here on the exciton-phonon coupling and role of trap states formed at the interface of structural dislocations in CdSe quantum dots (QDs) synthesized by kinetic growth method. Even though non-luminescing, our studies recognize their signatures in the temperature dependent photoluminescence characteristics of lowest QD excitonic state and have some useful implications for structural quality of thus synthesized QDs. We have explained the observed temperature dependence of PL intensity in terms of a simple model taking account of different radiative and nonradiative recombination processes as well as carrier trapping/detrapping and determined the depth of potential well formed due to such long range defects. Our studies indicate the presence of such defect states only in QD samples size sorted by aliquoting at intermediate intervals during the reaction and do not appear when the reaction proceeds uninterrupted.
关键词： Temperature dependent photoluminescence,Exciton-phonon coupling,Thermal escape,CdSe Quantum Dots
更新于2025-09-16 10:30:52
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-shell excitons studied using two-dimensional coherent spectroscopy
摘要： The dephasing mechanisms of p-shell and s-shell excitons in an InAs self-assembled quantum dot ensemble are examined using two-dimensional coherent spectroscopy (2DCS). 2DCS provides a comprehensive picture of how the energy level structure of dots affects the exciton dephasing rates and recombination lifetimes. We find that at low temperatures, dephasing of s-shell excitons is lifetime limited, whereas p-shell excitons exhibit significant pure dephasing due to scattering between degenerate spin states. At elevated temperatures, quadratic exciton-phonon coupling plays an important role in both s-shell and p-shell exciton dephasing. We show that multiple p-shell states are also responsible for stronger phonon dephasing for these transitions.
关键词： quantum dots,two-dimensional coherent spectroscopy,dephasing,InAs,exciton-phonon coupling
更新于2025-09-10 09:29:36
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Demonstration of resonant inelastic x-ray scattering as a probe of exciton-phonon coupling
摘要： Resonant inelastic x-ray scattering (RIXS) is a promising technique for obtaining electron-phonon coupling constants. However, the ability to extract these coupling constants throughout the Brillouin zone for crystalline materials remains limited. To address this need, we developed a Green’s function formalism to capture electron-phonon contributions to core-level spectroscopies without explicitly solving the full vibronic problem. Our approach is based on the cumulant expansion of the Green’s function combined with many-body theory calculated vibrational coupling constants. The methodology is applied to x-ray photoemission spectroscopy, x-ray absorption spectroscopy (XAS), and RIXS. In the case of the XAS and RIXS, we use a two-particle exciton Green’s function, which accounts implicitly for particle-hole interference effects that have previously proved difficult. To demonstrate the methodology and gain a deeper understanding of the experimental technique, we apply our formalism to small molecules, for which unambiguous experimental data exist. This comparison reveals that the vibronic coupling constant probed by RIXS is in fact related to exciton-phonon coupling rather than electron-phonon coupling, challenging the conventional interpretation of the experiment.
关键词： electron-phonon coupling,Green’s function formalism,exciton-phonon coupling,Resonant inelastic x-ray scattering,vibronic coupling
更新于2025-09-04 15:30:14