Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 19 de 19
Filtrar
1.
J Am Chem Soc ; 146(19): 13226-13235, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38700957

RESUMO

Strained carbon nanohoops exhibit attractive photophysical properties due to their unique π-conjugated structure. However, incorporation of such nanohoops into the pincer ligand of metal complexes has rarely been explored. Herein, a new family of highly strained cyclometalated platinum(II) nanohoops has been synthesized and characterized. Strain-promoted C-H bond activation has been observed during the metal coordination process, and Hückel-Möbius topology and random-columnar packing in the solid state are found. Transient absorption spectroscopy revealed the size-dependent excited state properties of the nanohoops. Moreover, the nanohoops have been successfully employed as active materials in the fabrication of solution-processable resistive memory devices, including the use of the smallest platinum(II) nanohoop for the fabrication of a binary memory, with low switching threshold voltages of ca. 1.5 V, high ON/OFF current ratios, and good stability. These results demonstrate that strain incorporation into the structure can be an effective strategy to fundamentally fine-tune the reactivity, optoelectronic, and resistive memory properties.

2.
J Am Chem Soc ; 146(37): 25589-25599, 2024 Sep 18.
Artigo em Inglês | MEDLINE | ID: mdl-39248725

RESUMO

Cross-linking strategies have found wide applications in chemical biology, enabling the labeling of biomolecules and monitoring of protein-protein interactions. Nitrone exhibits remarkable versatility and applicability in bioorthogonal labeling due to its high reactivity with strained alkynes via the strain-promoted alkyne-nitrone cycloaddition (SPANC) reaction. In this work, four cyclometalated iridium(III) polypyridine complexes functionalized with two nitrone units were designed as novel phosphorogenic bioorthogonal reagents for bioimaging and phototherapeutics. The complexes showed efficient emission quenching, which is attributed to an efficient nonradiative decay pathway via the low-lying T1/S0 minimum energy crossing point (MECP), as revealed by computational studies. However, the complexes displayed significant emission enhancement and lifetime extension upon reaction with (1R,8S,9s)-bicyclo[6.1.0]non-4-yne (BCN) derivatives. In particular, they showed a remarkably higher reaction rate toward a bis-cyclooctyne derivative (bis-BCN) compared with its monomeric counterpart (mono-BCN). Live-cell imaging and (photo)cytotoxicity studies revealed higher photocytotoxicity in bis-BCN-pretreated cells, which is ascribed to the enhanced singlet oxygen (1O2) photosensitization resulting from the elimination of the nitrone-associated quenching pathway. Importantly, the cross-linking properties and enhanced reactivity of the complexes make them highly promising candidates for the development of hydrogels and stapled/cyclized peptides, offering intriguing photophysical, photochemical, and biological properties. Notably, a nanosized hydrogel (2-gel) demonstrated potential as a drug delivery system, while a stapled peptide (2-bis-pDIKK) exhibited p53-Mdm2 inhibitory activity related to apoptosis and a cyclized peptide (2-bis-RGD) showed cancer selectivity.


Assuntos
Complexos de Coordenação , Irídio , Óxidos de Nitrogênio , Irídio/química , Óxidos de Nitrogênio/química , Óxidos de Nitrogênio/farmacologia , Complexos de Coordenação/química , Complexos de Coordenação/farmacologia , Complexos de Coordenação/síntese química , Humanos , Estrutura Molecular , Antineoplásicos/farmacologia , Antineoplásicos/química , Antineoplásicos/síntese química , Nanomedicina Teranóstica
3.
Small ; 20(12): e2307393, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-37897146

RESUMO

Described here are sterically hindered tetradentate [Pt(O^N^C^N)] emitters (Pt-1, Pt-2, and Pt-3) developed for stable and high-performance green phosphorescent organic light-emitting diodes (OLEDs). These Pt(II) emitters exhibit strong saturated green phosphorescence (λmax = 517-531 nm) in toluene and mCP thin films with emission quantum yields as high as 0.97, radiative rate constants (kr) as high as 4.4-5.3 × 105 s-1 and reduced excimer emission, and with a preferential horizontally oriented transition dipole ratio of up to 84%. Theoretical calculations show that p-(hetero)arene substituents at the periphery of the ligand scaffolds in Pt-1, Pt-2, and Pt-3 can i) enhance the spin-orbit coupling (SOC) between the lower singlet excited states and the T1 state, and S0→Sn (n = 1 or 2) transition dipole moment, and ii) introducing additional SOC activity and the bright 1ILCT[π(carbazole)→π*(N^C^N)] excited state (Pt-2 and Pt-3), which are the main contributors to the increased kr values. Utilizing these tetradentate Pt(II) emitters, green phosphorescent OLEDs are fabricated with narrow-band electroluminescence (FWHM down to 36 nm), high external quantum efficiency, current efficiency up to 27.6% and 98.7 cd A-1, and an unprecedented device lifetime (LT95) of up to 9270 h at 1000 cd m-2 under laboratory conditions.

4.
Angew Chem Int Ed Engl ; 63(6): e202316200, 2024 Feb 05.
Artigo em Inglês | MEDLINE | ID: mdl-38009456

RESUMO

Due to the ubiquity of chirality in nature, chiral self-assembly involving self-sorting behaviors has remained as one of the most important research topics of interests. Herein, starting from a racemic mixture of SEG-based (SEG=SEGPHOS) chlorogold(I) precursors, a unique chiral butterfly-shape hexadecanuclear gold(I) cluster (Au16 ) with different ratios of RSEG and SSEG ligands is obtained via homoleptic and heterochiral self-sorting. More interestingly, by employing different chlorogold(I) precursors of opposite chirality (such as RSEG -Au2 and SBIN -Au2 (BIN=BINAP)), an unprecedented heteroleptic and heterochiral self-sorting strategy has been developed to give a series of heteroleptic chiral decanuclear gold(I) clusters (Au10 ) with propellor-shape structures. Heterochiral and heteroleptic self-sorting have also been observed between enantiomers of homoleptic chiral Au10 clusters to result in the heteroleptic chiral Au10 clusters via cluster-to-cluster transformation. Incorporation of heteroleptic ligands is found to decrease the symmetry from S4 of homoleptic meso Au10 to C2 of heteroleptic chiral Au10 clusters. The chirality has been transferred from the axial chiral ligands and stored in the heteroleptic gold(I) clusters.

5.
J Am Chem Soc ; 145(44): 24098-24107, 2023 Nov 08.
Artigo em Inglês | MEDLINE | ID: mdl-37874942

RESUMO

We present a novel class of one-electron multi-channel molecular orbital images (MolOrbImages) designed for the prediction of excited-state energetics in conjunction with the state-of-the-art VGG-type machine-learning architecture. By representing hole and particle states in the excitation process as channels of MolOrbImages, the revised VGG model achieves excellent prediction accuracy for both low-lying singlet and triplet states, with mean absolute errors (MAEs) of <0.08 and <0.1 eV for QM9 molecules and large photofunctional materials with up to 560 atoms, respectively. Remarkably, the model demonstrates exceptional performance (MAE < 1 kcal/mol) for the T1 state of QM9 molecules, making it a non-system-specific model that approaches chemical accuracy. The general rules attained, for instance, the improved performance with well-defined MO energies and the reduced overfitting concern via the inclusion of physically insightful hole-particle information, provide invaluable guidelines for the further design of orbital-based descriptors targeting molecular excited states.

6.
Opt Lett ; 47(4): 758-761, 2022 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-35167518

RESUMO

A multicore fiber Bragg grating (MC-FBG) array shape sensor is a powerful tool for a variety of applications. However, the efficient fabrication of high-quality MC-FBG arrays remains a problem. Here, we report for the first time, to the best of our knowledge, a new method of directly writing FBG arrays in a seven-core fiber (SCF) through the protective coating using femtosecond laser auto-positioning point-by-point technology, which is accomplished by image recognition and micro-displacement compensation. An MC-FBG array consisting of 140 individual FBGs with a grating length of 2 mm was successfully inscribed into seven cores of a 440 mm-long SCF. Each core contained 20 wavelength-division-multiplexed (WDM) FBGs with wavelengths ranging from 1522.11 nm to 1579.28 nm. In other words, the MC-FBG array consisted of 20 WDM nodes with an interval of 2 cm along the fiber, and each node contained seven identical FBGs integrated in parallel into the fiber cross-section. Moreover, the fabricated MC-FBG array exhibited a strong orientation dependence in bend sensing, with a maximum sensitivity of 55.49 pm/m-1. Subsequently, 2D and 3D shape sensing were demonstrated using the fabricated MC-FBG array, with maximum reconstruction errors per unit length of 4.51% and 10.81%, respectively. Hence, the MC-FBG arrays fabricated using the proposed method are useful in many applications, such as posture monitoring, smart robotics, and minimally invasive surgery.

7.
J Chem Phys ; 156(21): 211101, 2022 Jun 07.
Artigo em Inglês | MEDLINE | ID: mdl-35676135

RESUMO

Probing chemical bonding in molecules containing lanthanide elements is of theoretical interest, yet it is computationally challenging because of the large valence space, relativistic effects, and considerable electron correlation. We report a high-level ab initio study that quantifies the many-body nature of Ce-O bonding with the coordination environment of the Ce center and particularly the roles of the 4f orbitals. The growing significance of the overlap between Ce 4f and O 2p orbitals with the increasing coordination of Ce atoms enhances Ce-O bond covalency and in return directs the molecular geometry. Upon partial reduction from neutral to anionic ceria, the excessive electrons populate the Ce-centered localized 4f orbital. The interplay between the admixture and localization of the 4f-block dually modulates bonding patterns of cerium oxide molecules, underlying the importance of many-body interactions between ligands and various lanthanide elements.

8.
Opt Lett ; 46(22): 5663-5666, 2021 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-34780431

RESUMO

The reflection spectra of conventional fiber Bragg gratings (FBGs) with uniform index modulation profiles typically have strong sidelobes, which hamper the performance of FBG-based optical filters, fiber lasers, and sensors. Here, we propose and demonstrate a femtosecond laser line-by-line (LbL) scanning technique for fabricating apodized FBGs with suppressed sidelobes. This approach can flexibly achieve various apodized modulation profiles via precise control over the length and/or transverse position of each laser-inscribed index modification track. We theoretically and experimentally studied the influences of the apodization function on the side-mode suppression ratio (SMSR) in the fabricated apodized FBG, and the results show that a maximum SMSR of 20.6 dB was achieved in a Gaussian-apodized FBG. Subsequently, we used this method to fabricate various apodized FBGs, and the SMSRs in these FBGs were reduced effectively. Specifically, a dense-wavelength-division-multiplexed Gaussian-apodized FBG array with a wavelength interval of 1.50 nm was successfully fabricated, and the SMSR in such an array is 14 dB. Moreover, a Gaussian-apodized phase-shifted FBG and chirped FBG were also demonstrated with a high SMSR of 14 and 16 dB, respectively. Therefore, such an apodization method based on a modified femtosecond laser LbL scanning technique is an effective and flexible way to fabricate various FBGs with high SMSRs, which is promising to improve the performance of optical filters, fiber lasers, and sensors.

9.
J Chem Phys ; 155(10): 104111, 2021 Sep 14.
Artigo em Inglês | MEDLINE | ID: mdl-34525813

RESUMO

We present a novel theory and implementation for computing coupled electronic and quantal nuclear subsystems on a single potential energy surface, moving beyond the standard Born-Oppenheimer (BO) separation of nuclei and electrons. We formulate an exact self-consistent nucleus-electron embedding potential from the single product molecular wavefunction and demonstrate that the fundamental behavior of the correlated nucleus-electron can be computed for mean-field electrons that are responsive to a quantal anharmonic vibration of selected nuclei in a discrete variable representation. Geometric gauge choices are discussed and necessary for formulating energy invariant biorthogonal electronic equations. Our method is further applied to characterize vibrationally averaged molecular bonding properties of molecular energetics, bond lengths, and protonic and electron densities. Moreover, post-Hartree-Fock electron correlation can be conveniently computed on the basis of nucleus-electron coupled molecular orbitals, as demonstrated for correlated models of second-order Møllet-Plesset perturbation and full configuration interaction theories. Our approach not only accurately quantifies non-classical nucleus-electron couplings for revising molecular bonding properties but also provides an alternative time-independent approach for deploying non-BO molecular quantum chemistry.

10.
Angew Chem Int Ed Engl ; 59(31): 12741-12745, 2020 07 27.
Artigo em Inglês | MEDLINE | ID: mdl-32343022

RESUMO

The chemical ligation of two unprotected peptides to generate a natural peptidic linkage specifically at the C- and N-termini is a desirable goal in chemical protein synthesis but is challenging because it demands high reactivity and selectivity (chemo-, regio-, and stereoselectivity). We report an operationally simple and highly effective chemical peptide ligation involving the ligation of peptides with C-terminal salicylaldehyde esters to peptides with N-terminal cysteine/penicillamine. The notable features of this method include its tolerance of steric hinderance from the side groups on either ligating terminus, thereby allowing flexible disconnection at sites that are otherwise difficult to functionalize. In addition, this method can be expanded to selective desulfurization and one-pot ligation-desulfurization reactions. The effectiveness of this method was demonstrated by the synthesis of VISTA (216-311), PD-1 (192-288) and Eglin C.


Assuntos
Cisteína/análogos & derivados , Penicilamina/análogos & derivados , Fragmentos de Peptídeos/síntese química , Aldeídos/química , Sequência de Aminoácidos , Receptor de Morte Celular Programada 1/química , Proteínas/síntese química
11.
J Sci Food Agric ; 98(3): 1061-1070, 2018 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-28722221

RESUMO

BACKGROUND: Rice husk is a complex hierarchical assembly of hollow fibers consisting of cellulose, hemicellulose and lignin. In addition, it can also contain pectin and significant amounts of silica. Rice husk can be used in diverse applications and generally in the form of rice husk powder. This study aimed to investigate the structural features and mechanical properties of various varieties of whole rice husks. RESULTS: Rice husk consists of three sections: epidermis, sub-hypodermis and hypodermis. The thickness of these layers, the diameters of the hollow fibers and the wall thickness vary with the variety of rice husk. The elastic modulus is typically between 0.3 and 2.6 GPa, and the ultimate tensile strength varies from 19 to 135 MPa depending on the variety of rice husk. CONCLUSION: Rice husk has a unique hierarchical structure in which the fibers exhibit a staggered perpendicular arrangement and the entire fiber sections are covered by an external shell. The tensile properties vary with the variety of rice husk. The wide range in these tensile properties may be attributed to the size and orientation of the fibers. © 2017 Society of Chemical Industry.


Assuntos
Oryza/química , Sementes/química , Celulose/química , Lignina/química , Oryza/classificação , Pectinas/química , Sementes/classificação , Resistência à Tração
12.
J Am Chem Soc ; 138(51): 16596-16599, 2016 12 28.
Artigo em Inglês | MEDLINE | ID: mdl-27992194

RESUMO

Biological entities, such as DNA bases or proteins, possess numerous tautomers and isomers that lie close in energy, making the experimental characterization of a unique tautomer challenging. We apply VUV synchrotron-based experiments combined with state-of-the-art ab initio methodology to determine the adiabatic ionization energies (AIEs) of specific gas-phase cytosine tautomers produced in a molecular beam. The structures and energetics of neutral and cationic cytosine tautomers were determined using explicitly correlated methods. The experimental spectra correspond to well-resolved bands that are attributable to the specific contributions of five neutral tautomers of cytosine prior to ionization. Their AIEs are experimentally determined for the first time with an accuracy of 0.003 eV. This study also serves as an important showcase for other biological entities presenting a dense pattern of isomeric and tautomeric forms in their spectra that can be investigated to understand the charge redistribution in these species upon ionization.


Assuntos
Citosina/química , Fótons , Isomerismo , Processos Fotoquímicos
13.
Materials (Basel) ; 17(7)2024 Mar 25.
Artigo em Inglês | MEDLINE | ID: mdl-38612001

RESUMO

In the present work, the hot deformation behavior and microstructural evolution of a TiB2/Al-Zn-Mg-Cu-Zr composite were studied. Hot compression tests were conducted within a temperature range of 370 °C to 490 °C and a strain rate of 0.001 s-1 to 10 s-1. We established the Arrhenius constitutive equation with Zener-Hollomon parameters and processing maps and discussed the microstructural evolution during hot deformation. The results indicated that the safe processing parameter region falls within 370 °C-490 °C and 0.001 s-1-0.025 s-1. The influence of the strain rate on the safe processing range is more dominant than that of deformation temperature, which is primarily attributed to TiB2. Dynamic softening is primarily governed by dynamic recovery (DRV). Small particles (η, Al3Zr) can pin dislocations, promoting the rearrangement and annihilation of dislocations and facilitating DRV. Higher temperatures and lower strain rates facilitated dynamic recrystallization (DRX). Continuous dynamic recrystallization (CDRX) occurs near high-angle grain boundaries induced by strain-induced boundary migration (SIBM). TiB2 and large second-phase particles generate high-density geometrically necessary dislocations (GNBs) during hot deformation, which serve as nucleation sites for discontinuous dynamic recrystallization (DDRX). This enhances dynamic softening and improves formability.

14.
Artigo em Inglês | MEDLINE | ID: mdl-38292140

RESUMO

Purpose: To investigate the value of apolipoprotein A1 (ApoA1), apolipoprotein B (ApoB), and ApoA1/B ratio in pathogenic diagnosis of chronic obstructive pulmonary disease (COPD) complicated by acute lower respiratory tract infection, assisting comprehensive disease assessment. Patients and Methods: The study enrolled 171 COPD patients with acute lower respiratory tract infections, 35 COPD patients without acute lower respiratory tract infections, and 41 healthy controls. Correlation analysis and binary logistic regression were used to assess the roles of various factors in COPD with acute lower respiratory tract infections. Receiver operating characteristic (ROC) curves were plotted and area under curves (AUC) values were calculated to evaluate the predictive performance. Results: Infections were the cause of alterations in ApoA1, ApoB and ApoA1/B index. In correlation analysis for pathogenic diagnosis of COPD complicated by acute lower respiratory infections, age, ApoA1, ApoA1/B ratio, lymphocyte count (LYMPH), neutrophil count (NEUT), C-reactive protein (CRP), erythrocyte sedimentation rate (ESR) and endotoxin were significantly correlated. For predicting COPD complicated by acute lower respiratory tract bacterial infection, ApoA1 had the highest area under the ROC curve (AUC: 0.889), with sensitivity and specificity of 82.9% and 83.9%, respectively. The combination of NEUT and ApoA1 improved the prediction efficacy (AUC: 0.909; sensitivity/specificity: 85.1%/85.7%). Conclusion: ApoA1, ApoB, and ApoA1/B ratio are good indicators for predicting pathogens in COPD complicated by acute lower respiratory tract infection, especially ApoA1 which has high predictive value.


Assuntos
Doença Pulmonar Obstrutiva Crônica , Infecções Respiratórias , Humanos , Apolipoproteína A-I , Apolipoproteínas B , Biomarcadores , Estudos Transversais , Doença Pulmonar Obstrutiva Crônica/complicações , Doença Pulmonar Obstrutiva Crônica/diagnóstico , Infecções Respiratórias/diagnóstico
15.
Chem Sci ; 15(22): 8545-8556, 2024 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-38846386

RESUMO

A new class of amphiphilic tetradentate platinum(ii) Schiff base complexes has been designed and synthesized. The self-assembly properties by exploiting the potential Pt⋯Pt interactions of amphiphilic platinum(ii) Schiff base complexes in the solution state have been systematically investigated. The presence of Pt⋯Pt interactions has further been supported by computational studies and non-covalent interaction (NCI) analysis of the dimer of the complex. The extent of the non-covalent Pt⋯Pt and π-π interactions could be regulated by a variation of the solvent compositions and the hydrophobicity of the complexes, which is accompanied by attractive spectroscopic and luminescence changes and leads to diverse morphological transformations. The present work represents a rare example of demonstration of directed cooperative assembly of amphiphilic platinum(ii) Schiff base complexes by intermolecular Pt⋯Pt interactions in solution with an in-depth mechanistic investigation, providing guiding principles for the construction of supramolecular structures with desirable properties using platinum(ii) Schiff base building blocks.

16.
Chem Sci ; 15(31): 12606-12615, 2024 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-39118634

RESUMO

Achieving both high efficiency and high stability in blue thermally activated delayed fluorescence organic light-emitting diodes (TADF-OLEDs) is challenging for practical displays and lighting. Here, we have successfully developed a series of sky-blue to pure-blue emitting donor-acceptor (D-A) type TADF materials featuring a four-coordinated boron with 2,2'-(pyridine-2,6-diyl)diphenolate (dppy) ligands, i.e.1-8. Synergistic engineering of substituents on the phenyl bridge as well as the electronic properties and the attached positions of heteroatom N-donors not only enables fine-tuning of the emission colors, but also modulates the nature and energies of their triplet excited states that are important for the reverse intersystem crossing (RISC). Particularly for the compound with two methyl substituents on the phenyl bridge (compound 8), RISC is significantly facilitated through the vibronic coupling of the energetically close-lying triplet charge transfer (3CT) and the triplet local excited (3LE) states, when compared to analogue 7. Efficient sky-blue to pure-blue OLEDs with electroluminescence peaks (λ EL) at 460-492 nm have been obtained, in which ca. five-fold higher external quantum efficiencies (EQEs) of 18.9% have been demonstrated by 8 than that by 7. Moreover, ca. thirty times longer device operational half-lifetimes (LT50) of 9113 hours for 8 than that for 7 as well as satisfactory LT50 reaching 26 643 hours for 6 at an initial luminance of 100 cd m-2 have also been demonstrated. To the best of our knowledge, these results represent one of the best high-performance blue OLEDs based on tetracoordinated boron TADF emitters. Moreover, the design strategy presented here has provided an attractive strategy for enhancing the device performance of blue TADF-OLEDs.

17.
J Phys Chem Lett ; 14(7): 1955-1961, 2023 Feb 23.
Artigo em Inglês | MEDLINE | ID: mdl-36787423

RESUMO

We present a general machine learning framework for probing the electronic state properties using the novel quantum descriptor MolOrbImage. Each pixel of the MolOrbImage records the quantum information generated by the integration of the physical operator with a pair of bra and ket molecular orbital (MO) states. Inspired by the success of deep convolutional neural networks (NNs) in computer vision, we have implemented the convolutional-layer-dominated MO-NN model. Using the orbital energy and electron repulsion integral MolOrbImages, the MO-NN model achieves promising prediction accuracies against the ADC(2)/cc-pVTZ reference for transition energies to both low-lying singlet [mean absolute error (MAE) < 0.16 eV] and triplet (MAE < 0.14 eV) states. An apparent improvement in the prediction of oscillator strength, which has been shown to be challenging previously, has been demonstrated in this study. Moreover, the transferability test indicates the remarkable extrapolation capacity of the MO-NN model to describe the out of data set systems.

18.
Materials (Basel) ; 16(12)2023 Jun 13.
Artigo em Inglês | MEDLINE | ID: mdl-37374530

RESUMO

Nanocrystalline (NC) structure can lead to the considerable strengthening of metals and alloys. Obtaining appropriate comprehensive mechanical properties is always the goal of metallic materials. Here, a nanostructured Al-Zn-Mg-Cu-Zr-Sc alloy was successfully processed by high-pressure torsion (HPT) followed by natural aging. The microstructures and mechanical properties of the naturally aged HPT alloy were analyzed. The results show that the naturally aged HPT alloy primarily consists of nanoscale grains (~98.8 nm), nano-sized precipitates (20-28 nm in size), and dislocations (1.16 × 1015 m-2), and exhibits a high tensile strength of 851 ± 6 MPa and appropriate elongation of 6.8 ± 0.2%. In addition, the multiple strengthening modes that were activated and contributed to the yield strength of the alloy were evaluated according to grain refinement strengthening, precipitation strengthening, and dislocation strengthening, and it is shown that grain refinement strengthening and precipitation strengthening are the main strengthening mechanisms. The results of this study provide an effective pathway for achieving the optimal strength-ductility match of materials and guiding the subsequent annealing treatment.

19.
J Am Soc Mass Spectrom ; 32(3): 815-824, 2021 Mar 03.
Artigo em Inglês | MEDLINE | ID: mdl-33555854

RESUMO

The characterization of photoexcited electrons on the surface of nanomaterial remains challenging. Herein, laser excitation mass spectrometry combined with a chemical thermometer and electron acceptor has been developed to characterize the energetics and population density of photoexcited electrons transferred from gold nanoparticles (AuNPs). In contrast to laser fluence and bias voltage, the hot spots of closely packed AuNPs play a more significant role in enhancing the average energetics of photoexcited electrons, which can be harvested effectively by the electron acceptor. By harvesting more energetic photoexcited electrons for the desorption and ionization process, it is anticipated that the sensitive detection of biomarkers can be achieved, which is beneficial to metabolomic studies and early disease diagnosis.

SELEÇÃO DE REFERÊNCIAS
DETALHE DA PESQUISA