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1.
J Am Chem Soc ; 146(3): 1874-1886, 2024 Jan 24.
Artigo em Inglês | MEDLINE | ID: mdl-38085547

RESUMO

Photoluminescence (PL) imaging has broad applications in visualizing biological activities, detecting chemical species, and characterizing materials. However, the chemical information encoded in the PL images is often limited by the overlapping emission spectra of chromophores. Here, we report a PL microscopy based on the nonlinear interactions between mid-infrared and visible excitations on matters, which we termed MultiDimensional Widefield Infrared-encoded Spontaneous Emission (MD-WISE) microscopy. MD-WISE microscopy can distinguish chromophores that possess nearly identical emission spectra via conditions in a multidimensional space formed by three independent variables: the temporal delay between the infrared and the visible pulses (t), the wavelength of visible pulses (λvis), and the frequencies of the infrared pulses (ωIR). This method is enabled by two mechanisms: (1) modulating the optical absorption cross sections of molecular dyes by exciting specific vibrational functional groups and (2) reducing the PL quantum yield of semiconductor nanocrystals, which was achieved through strong field ionization of excitons. Importantly, MD-WISE microscopy operates under widefield imaging conditions with a field of view of tens of microns, other than the confocal configuration adopted by most nonlinear optical microscopies, which require focusing the optical beams tightly. By demonstrating the capacity of registering multidimensional information into PL images, MD-WISE microscopy has the potential of expanding the number of species and processes that can be simultaneously tracked in high-speed widefield imaging applications.

2.
Angew Chem Int Ed Engl ; : e202405123, 2024 May 07.
Artigo em Inglês | MEDLINE | ID: mdl-38714495

RESUMO

In this work, we investigate trion dynamics occurring at the heterojunction between organometallic molecules and a monolayer transition metal dichalcogenide (TMD) with transient electronic sum frequency generation (tr-ESFG) spectroscopy. By pumping at 2.4 eV with laser pulses, we have observed an ultrafast hole transfer, succeeded by the emergence of charge-transfer trions. This observation is facilitated by the cancellation of ground state bleach and stimulated emission signals due to their opposite phases, making tr-ESFG especially sensitive to the trion formation dynamics. The presence of charge-transfer trion at molecular functionalized TMD monolayers suggests the potential for engineering the local electronic structures and dynamics of specific locations on TMDs and offers a potential for transferring unique electronic attributes of TMD to the molecular layers.

3.
Proc Natl Acad Sci U S A ; 117(38): 23385-23392, 2020 09 22.
Artigo em Inglês | MEDLINE | ID: mdl-32907936

RESUMO

Understanding hydrogen-bond interactions in self-assembled lattice materials is crucial for preparing such materials, but the role of hydrogen bonds (H bonds) remains unclear. To gain insight into H-bond interactions at the materials' intrinsic spatial scale, we investigated ultrafast H-bond dynamics between water and biomimetic self-assembled lattice materials (composed of sodium dodecyl sulfate and ß-cyclodextrin) in a spatially resolved manner. To accomplish this, we developed an infrared pump, vibrational sum-frequency generation (VSFG) probe hyperspectral microscope. With this hyperspectral imaging method, we were able to observe that the primary and secondary OH groups of ß-cyclodextrin exhibit markedly different dynamics, suggesting distinct H-bond environments, despite being separated by only a few angstroms. We also observed another ultrafast dynamic reflecting a weakening and restoring of H bonds between bound water and the secondary OH of ß-cyclodextrin, which exhibited spatial uniformity within self-assembled domains, but heterogeneity between domains. The restoration dynamics further suggest heterogeneous hydration among the self-assembly domains. The ultrafast nature and meso- and microscopic ordering of H-bond dynamics could contribute to the flexibility and crystallinity of the material--two critically important factors for crystalline lattice self-assemblies--shedding light on engineering intermolecular interactions for self-assembled lattice materials.

4.
J Phys Chem Lett ; 13(37): 8733-8739, 2022 Sep 22.
Artigo em Inglês | MEDLINE | ID: mdl-36095150

RESUMO

Direct charge transfer at wet-processed organic/organic heterojunction interfaces is observed using femtosecond interfacial sensitive spectroscopy. UV-vis absorption and ultraviolet photoelectron spectroscopy both indicate that a new interfacial energy gap (∼1.2 eV) exists when an interface is formed between regioregular poly(3-hexylthiophene-2,5-diyl) and poly(benzimidazobenzophenanthroline). Resonant pumping at 1.2 eV creates an electric field-induced second-order optical signal, suggesting the existence of a transient electric field due to separated electrons and holes at interfaces, which recombine through a nongeminate process. The fact that direct charge transfer exists at wet-processed organic/organic heterojunctions provides a physical foundation for the previously reported ground-state charge transfer phenomenon. Also, it creates new opportunities to better control charge transfer with preserved momentum and spins at organic material interfaces for spintronic applications.

5.
Zhongguo Yi Liao Qi Xie Za Zhi ; 29(1): 5-6, 2005 Jan.
Artigo em Chinês | MEDLINE | ID: mdl-15875682

RESUMO

Some research on intelligent non-invasive temporary pacemakers is introduced in this paper. An industrial computer, some IC chips and other elements are used to construct its hardware, and its software is in C++ language. The experimental device has some intelligent functions of recognizing some arrhythmia. The system has a pacemaker module and an ECG monitor module. Its software includes a main program, a RS-232C communication program, a printer VxD, a pacing control VxD and ECG signal pretreatment and recognizing program and so on. The pacing-generating circuit is employed to make the precision control of pacing current. The communication between industrial-computer system and ECG module is completed through the DLL. The real time processing of ECG signals is based on filter method for a higher recognizing ratio. The system calculates several parameters to recognize certain arrhythmia and uses MIT/BIH database to validate the reliability of ECG recognition.


Assuntos
Arritmias Cardíacas/terapia , Inteligência Artificial , Marca-Passo Artificial , Processamento de Sinais Assistido por Computador/instrumentação , Design de Software , Algoritmos , Arritmias Cardíacas/diagnóstico , Ecocardiografia , Desenho de Equipamento , Humanos , Marca-Passo Artificial/classificação
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