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Ma, Xuedan

Publications and source records attributed to Ma, Xuedan.

45 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Reaching 90% Photoluminescence Quantum Yield in One-Dimensional Metal Halide C 4 N 2 H 14 PbBr 4 by Pressure-Suppressed Nonradiative Loss

Low-dimensional perovskite-related metal halides have emerged as a new class of light-emitting materials with tunable broadband emission from self-trapped excitons (STEs). Although various types of low-dimensional structures have been developed, fundamental understating of the structure–property relationships for this class of materials is still very limited, and further improvement of their optical properties remains greatly important. Here, we report a significant pressure-induced photoluminescence (PL) enhancement in a one-dimensional hybrid metal halide C 4 N 2 H 14 PbBr 4 , and the underlying mechanisms are investigated using in situ experimental characterization and first-principles calculations. Under a gigapascal pressure scale, the PL quantum yields (PLQYs) were quantitatively determined to show a dramatic increase from the initial value of 20% at ambient conditions to over 90% at 2.8 GPa. With in situ characterization of photophysical properties and theoretical analysis, we found that the PLQY enhancement was mainly attributed to the greatly suppressed nonradiative decay. Pressure can effectively tune the energy level of self-trapped states and increase the exciton binding energy, which leads to a larger Stokes shift. The resulting highly localized excitons with stronger binding reduce the probability for carrier scattering, to result in the significantly suppressed nonradiative decay. Overall, our findings clearly show that the characteristics of STEs in low-dimensional metal halides can be well-tuned by external pressure, and enhanced optical properties can be achieved.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

The Effect of Periodic Spatial Perturbations on the Emission Rates of Quantum Dots near Graphene Platforms

The quenching of fluorescence (FL) at the vicinity of conductive surfaces and, in particular, near a 2-D graphene layer has become an important biochemical sensing tool. The quenching is attributed to fast non-radiative energy transfer between a chromophore (here, a Quantum Dot, QD) and the lossy graphene layer. Increased emission rate is also observed when the QD is coupled to a resonator. Here, we combine the two effects in order to control the emission lifetime of the QD. In our case, the resonator was defined by an array of nano-holes in the oxide substrate underneath a graphene surface guide. At resonance, the surface mode of the emitted radiation is concentrated at the nano-holes. Thus, the radiation of QD at or near the holes is spatially correlated through the hole-array’s symmetry. We demonstrated an emission rate change by more than 50% as the sample was azimuthally rotated with respect to the polarization of the excitation laser. In addition to an electrical control, such control over the emission lifetime could be used to control Resonance Energy Transfer (RET) between two chromophores.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Strain-Induced Trapping of Indirect Excitons in MoSe 2 /WSe 2 Heterostructures

Understanding and control of excitons in transition metal dichalcogenide (TMD) materials are essential for the exploration of the rich many-body physics in TMDs and their applications in photonic and optoelectronic devices. Local strain modulation has been utilized as an effective approach for creating potential traps and localizing intralayer excitons in TMD monolayers. Here, we investigate the effect of strains on indirect excitons in TMD heterostructures. The emergence of narrow spectral peaks from the strained sites together with their drastically reduced lifetimes indicates the formation of potential traps in the heterostructures and the trapping of indirect excitons in them. The absence of photon-antibunching from these trapped indirect excitons further reveals their weak localization in the potential traps. Here, our study indicates that, compared to the case of intralayer excitons, narrower potential traps are required for obtaining highly localized indirect excitons due to their unique properties. These findings have important implications for creating long-wavelength quantum emitters in TMD heterostructures and the exploration of indirect exciton condensation and motion in TMDs.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Ultrasonication-assisted trace amount solvent synthesis of Cs 4 PbBr 6 crystal with ultra-bright green light emission

Cs 4 PbBr 6 crystals have been synthesized by an ultrasonication-assisted trace amount polar solvent method. The prepared green Cs 4 PbBr 6 material was found to have high photoluminescence (PL) brightness and 10 ns PL lifetime. The prepared green light emitting device can achieve the maximum brightness of 3.8 × 10 9 cd/m 2 , which is nearly 100 times higher than a wick. The white light emitting device based on Cs 4 PbBr 6 crystals has better performance than commercial products, which can cover 32.3% of the color gamut and achieves 107.3% coverage for International Commission on Illumination (CIE)1931 and 84.8% coverage for CIE1976.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Creation of Single-Photon Emitters in WSe 2 Monolayers Using Nanometer-Sized Gold Tips

Due to their tunable bandgaps and strong spin-valley locking, transition metal dichalcogenides constitute a unique platform for hosting single-photon emitters. Here, we present a versatile approach for creating bright single-photon emitters in WSe 2 monolayers by the deposition of gold nanostars. Our molecular dynamics simulations reveal that the formation of the quantum emitters is likely caused by the highly localized strain fields created by the sharp tips of the gold nanostars. The surface plasmon modes supported by the gold nanostars can change the local electromagnetic fields in the vicinity of the quantum emitters, leading to their enhanced emission intensities. Moreover, by correlating the emission energies and intensities of the quantum emitters, we are able to associate them with two types of strain fields and derive the existence of a low-lying dark state in their electronic structures. The findings here are highly relevant for the development and understanding of single-photon emitters in transition metal dichalcogenide materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Bright trion emission from semiconductor nanoplatelets

The trion, a quasiparticle comprising one exciton and an additional charge carrier, offers unique opportunities for generating spin-photon interfaces that can be used in developing quantum networks. Trions are also actively sought after for integrated optoelectronic devices including photovoltaics, photodetectors, and spintronics. However, formation of trions in strongly confined low-dimensional materials is often deemed detrimental. This is because trion emission in such materials is typically prohibited due to the predominant nonradiative Auger recombination processes. Semiconductor nanoplatelets with their strong confinement in the thickness direction and extended lateral geometries exhibit large exciton coherence sizes and reduced carrier-carrier interactions that may enable unprecedented trion properties. In this paper, we perform optical spectroscopic studies of individual CdSe nanoplatelets at cryogenic temperatures and observe bright trion emission with intensities comparable to that of neutral exciton emission. We perform carrier dynamics studies of the nanoplatelets and find that due to their extended lateral geometry, the fast radiative decay rate of the nanoplatelets at cryogenic temperatures is comparable to the inhibited Auger recombination rate, leading to the bright trion emission. Our tight-binding theory further reveals distinct size-tunable trion emission in the nanoplatelets that is advantageous for efficient trion emission. These properties make semiconductor nanoplatelets potential candidates as photon sources for optoelectronic and quantum logic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Accelerating quantum optics experiments with statistical learning

Quantum optics experiments, involving the measurement of low-probability photon events, are known to be extremely time-consuming. We present a methodology for accelerating such experiments using physically motivated ansatzes together with simple statistical learning techniques such as Bayesian maximum a posteriori estimation based on few-shot data. We show that it is possible to reconstruct time-dependent data using a small number of detected photons, allowing for fast estimates in under a minute and providing a one-to-two order of magnitude speed-up in data acquisition time. We test our approach using real experimental data to retrieve the second order intensity correlation function, G (2) ($τ$), as a function of time delay τ between detector counts, for thermal light as well as anti-bunched light emitted by a quantum dot driven by periodic laser pulses. The proposed methodology has a wide range of applicability and has the potential to impact the scientific discovery process across a multitude of domains.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Large-Scale Plasmonic Hybrid Framework with Built-In Nanohole Array as Multifunctional Optical Sensing Platforms

Light coupling with patterned subwavelength hole arrays induces enhanced transmission supported by the strong surface plasmon mode. In this work, a nanostructured plasmonic framework with vertically built-in nanohole arrays at deep-subwavelength scale (6 nm) is demonstrated using a two-step fabrication method. The nanohole arrays are formed first by the growth of a high-quality two-phase (i.e., Au–TiN) vertically aligned nanocomposite template, followed by selective wet-etching of the metal (Au). Such a plasmonic nanohole film owns high epitaxial quality with large surface coverage and the structure can be tailored as either fully etched or half-way etched nanoholes via careful control of the etching process. The chemically inert and plasmonic TiN plays a role in maintaining sharp hole boundary and preventing lattice distortion. Optical properties such as enhanced transmittance and anisotropic dielectric function in the visible regime are demonstrated. Numerical simulation suggests an extended surface plasmon mode and strong field enhancement at the hole edges. Furthermore, two demonstrations, including the enhanced and modulated photoluminescence by surface coupling with 2D perovskite nanoplates and the refractive index sensing by infiltrating immersion liquids, suggest the great potential of such plasmonic nanohole array for reusable surface plasmon-enhanced sensing applications.

42 ENGINEERING↗