Effects of crystallographic facet-specific peptide adsorption along single ZnO nanorods on the characteristic fluorescence intensification on nanorod ends (FINE) phenomenon

Singh, Manpreet; Zhuo, Xiaolu; Choi, Daniel S.; Gonzalez, Lorelis E.; Wang, Jianfang; Hahm, Jong‐in

doi:10.1039/c5nr05354d

Cited by 8 publications

(13 citation statements)

References 39 publications

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“…The fluorescence panel in Figure 2(A) with all polarizations allowed during excitation and collection clearly shows the characteristic FINE phenomenon we have previously reported. 10,11,15,28,43 The unique behavior of FINE originates from the coupled and waveguided emission from the fluorophores placed on top of the ZnO NR which travels through the NR via the mechanisms of subwavelength waveguiding and surface evanescent wave propagation. 10,11,28 This optical signal is highly intensified and spatially localized at the NR termini, as clearly displayed in the fluorescence intensity graph plotted as a function of the position along the long axis of the NR in the right panel of Figure 2(A).…”

Section: Resultsmentioning

confidence: 99%

“…10,11,14,28 When examining the temporal and spatial characteristics of enhanced biomolecular fluorescence on individual ZnO NRs, we found that both the signal intensity and photostability along the NR length show strikingly different profiles relative to those on conventional polymeric platforms. 10,11,29 Unlike the spatially uniform signal observed on polymers, both the magnitude and temporal stability of the fluorescence signal from fluorophore-coupled biomolecules on ZnO NRs were not only much increased relative to those on polymers but also highly intensified at the NR ends relative to the NR main body.…”

Section: Introductionmentioning

confidence: 98%

“…This effect was later revealed to stem from the fact that the fluorophore-emitted signals are effectively guided as surface evanescent waves along the NR and through the optical cavity of the subwavelength-waveguiding ZnO NR medium before they are finally radiated out to the far field from the two NR ends. 10,11,28 We have subsequently determined various nanomaterial- and biomolecule-related factors influencing the degree of FINE ( DoF ). 10,11,28 The DoF serves as a measure of the degree of signal enhancement at ZnO NR ends with respect to the NR middle.…”

Section: Introductionmentioning

confidence: 99%

“…10,11,28 We have subsequently determined various nanomaterial- and biomolecule-related factors influencing the degree of FINE ( DoF ). 10,11,28 The DoF serves as a measure of the degree of signal enhancement at ZnO NR ends with respect to the NR middle. DoF is the ratio quantified as the difference in the average fluorescence intensity measured at the end versus the middle of the NR divided by the average intensity measured on the main body.…”

Section: Introductionmentioning

confidence: 99%

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Polarization-resolved mechanistic investigation of fluorescence signal intensification on zinc oxide nanorod ends

et al. 2017

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The superior optical properties of zinc oxide nanorods (ZnO NRs) have continued to promote their broad use in photonic, photoelectric, light detecting, and biosensing applications. One particularly important property pertinent to biodetection is fluorescence intensification on nanorods ends (FINE), a phenomenon in which highly spatially localized and strongly intensified fluorescence signal with its extended photostability at the NR ends is seen from the emission profiles of fluorophore-coupled biomolecules on ZnO NRs. Therefore, understanding key parameters affecting the FINE phenomenon and the degree of FINE (DoF) is critical for their applications in biosensors. In this study, we describe in detail the outcomes of polarization-resolved measurements by systematically considering the polarization effects on FINE and DoF as a function of NR tilt angle and position along the NR. Specifically, we elucidate the exact roles of the different states of light polarization in FINE and quantitatively determine the explicit contributions arising from distinctive polarization states to the DoF. We confirm that the presence of the FINE phenomenon is ubiquitous from the fluorophore-coupled ZnO NR systems, regardless of the polarization setting. We subsequently show that DoF is significantly affected by the light-matter interaction geometry. We reveal the specific polarization conditions that contribute dominantly to the FINE effect. The highest DoF from a NR and the greatest NR end intensity can be achieved when both the excitation and collection polarization states are perpendicular to the NR main axis. Insights from this study provide valuable design principles for selecting the polarization state and light-matter interaction geometry to attain maximum FINE as well as DoF on ZnO NRs. The precise understanding of polarization-derived consequences on FINE and DoF manifested differently as a function of position on individual NRs can be also important for warranting accurate interpretation and quantification of the position-dependent, fluorophore-emitted signals on single ZnO NRs. Hence, our findings from this study can be extremely beneficial in fluorescence-based sensing and detection settings utilizing polarization.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 98%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Polarization-resolved mechanistic investigation of fluorescence signal intensification on zinc oxide nanorod ends

et al. 2017

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“…We have previously demonstrated that ZnO NRs can be successfully employed in bioanalyte detection [ 12 , 13 , 14 , 29 , 30 , 31 , 32 , 33 ]. In these efforts, pristine ZnO NRs served as efficient subwavelength waveguides and surface evanescent wave carriers, which subsequently permitted ultrasensitive detection of DNA- and protein-derived fluorescence signals.…”

Section: Introductionmentioning

confidence: 99%

Spatially Correlated, Single Nanomaterial-Level Structural and Optical Profiling of Cu-Doped ZnO Nanorods Synthesized via Multifunctional Silicides

et al. 2018

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We demonstrate a straightforward and effective method to synthesize vertically oriented, Cu-doped ZnO nanorods (NRs) using a novel multipurpose platform of copper silicide nanoblocks (Cu3Si NBs) preformed laterally in well-defined directions on Si. The use of the surface-organized Cu3Si NBs for ZnO NR growth successfully results in densely assembled Cu-doped ZnO NRs on each NB platform, whose overall structures resemble thick bristles on a brush head. We show that Cu3Si NBs can uniquely serve as a catalyst for ZnO NRs, a local dopant source of Cu, and a prepatterned guide to aid the local assembly of the NRs on the growth substrate. We also ascertain the crystalline structures, optical properties, and spectroscopic signatures of the Cu-doped ZnO NRs produced on the NBs, both at each module of NRs/NB and at their ensemble level. Subsequently, we determine their augmented properties relative to the pristine form of undoped ZnO NRs and the source material of Cu3Si NBs. We provide spatially correlated structural and optical data for individual modules of Cu-doped ZnO NRs assembled on a Cu3Si NB by resolving them along the different positions on the NB. Ensemble-averaged versus individual behaviors of Cu-doped ZnO NRs on Cu3Si NBs are then compared. We further discuss the potential impact of such ZnO-derived NRs on their relatively unexplored biological and biomedical applications. Our efforts will be particularly useful when exploiting each integrated module of self-aligned, Cu-doped ZnO NRs on a NB as a discretely addressable, active element in solid-state sensors and miniaturized luminescent bioprobes.

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Strong Structural and Electronic Binding of Bovine Serum Albumin to ZnO via Specific Amino Acid Residues and Zinc Atoms

2021

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ZnO biointerfaces with serum albumin have attracted noticeable attention due to the increasing interest in developing ZnO‐based materials for biomedical applications. ZnO surface morphology and chemistry are expected to play a critical role on the structural, optical, and electronic properties of albumin‐ZnO complexes. Yet there are still large gaps in the understanding of these biological interfaces. Herein we comprehensively elucidate the interactions at such interfaces by using atomic force microscopy and nanoshaving experiments to determine roughness, thickness, and adhesion properties of BSA layers adsorbed on the most typical polar and non‐polar ZnO single‐crystal facets. These experiments are corroborated by force field (FF) and density‐functional tight‐binding (DFTB) calculations on ZnO‐BSA interfaces. We show that BSA adsorbs on all the studied ZnO surfaces while interactions of BSA with ZnO are found to be considerably affected by the atomic surface structure of ZnO. BSA layers on the (0001‾) surface have the highest roughness and thickness, hinting at a specific upright BSA arrangement. BSA layers on (101‾0) surface have the strongest binding, which is well correlated with DFTB simulations showing atomic rearrangement and bonding between specific amino acids (AAs) and ZnO. Besides the structural properties, the ZnO interaction with these AAs also controls the charge transfer and HOMO‐LUMO energy positions in the BSA‐ZnO complexes. This ZnO facet‐specific protein binding and related structural and electronic effects can be useful for improving the design and functionality of ZnO‐based materials and devices.

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Effects of crystallographic facet-specific peptide adsorption along single ZnO nanorods on the characteristic fluorescence intensification on nanorod ends (FINE) phenomenon

Cited by 8 publications

References 39 publications

Polarization-resolved mechanistic investigation of fluorescence signal intensification on zinc oxide nanorod ends

Polarization-resolved mechanistic investigation of fluorescence signal intensification on zinc oxide nanorod ends

Spatially Correlated, Single Nanomaterial-Level Structural and Optical Profiling of Cu-Doped ZnO Nanorods Synthesized via Multifunctional Silicides

Strong Structural and Electronic Binding of Bovine Serum Albumin to ZnO via Specific Amino Acid Residues and Zinc Atoms

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