Browsing by Author "Neumann, Oara"
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Item Au Nanomatryoshkas as Efficient Near-Infrared Photothermal Transducers for Cancer Treatment: Benchmarking against Nanoshells(American Chemical Society, 2014) Ayala-Orozco, Ciceron; Urban, Cordula; Knight, Mark W.; Urban, Alexander Skyrme; Neumann, Oara; Bishnoi, Sandra W.; Mukherjee, Shaunak; Goodman, Amanda M.; Charron, Heather; Mitchell, Tamika; Shea, Martin; Roy, Ronita; Nanda, Sarmistha; Schiff, Rachel; Halas, Naomi J.; Joshi, AmitAu nanoparticles with plasmon resonances in the near-infrared (NIR) region of the spectrum efficiently convert light into heat, a property useful for the photothermal ablation of cancerous tumors subsequent to nanoparticle uptake at the tumor site. A critical aspect of this process is nanoparticle size, which influences both tumor uptake and photothermal efficiency. Here, we report a direct comparative study of ∼90 nm diameter Au nanomatryoshkas (Au/SiO2/Au) and ∼150 nm diameter Au nanoshells for photothermal therapeutic efficacy in highly aggressive triple negative breast cancer (TNBC) tumors in mice. Au nanomatryoshkas are strong light absorbers with 77% absorption efficiency, while the nanoshells are weaker absorbers with only 15% absorption efficiency. After an intravenous injection of Au nanomatryoshkas followed by a single NIR laser dose of 2 W/cm2 for 5 min, 83% of the TNBC tumor-bearing mice appeared healthy and tumor free >60 days later, while only 33% of mice treated with nanoshells survived the same period. The smaller size and larger absorption cross section of Au nanomatryoshkas combine to make this nanoparticle more effective than Au nanoshells for photothermal cancer therapy.Item Compact solar autoclave based on steam generation using broadband light-harvesting nanoparticles(National Academy of Sciences, 2013) Neumann, Oara; Feronti, Curtis; Neumann, Albert D.; Dong, Anjie; Schell, Kevin; Lu, Benjamin; Kim, Eric; Quinn, Mary; Thompson, Shea; Grady, Nathaniel; Nordlander, Peter; Oden, Maria; Halas, Naomi J.; Laboratory for Nanophotonics; Rice Quantum InstituteThe lack of readily available sterilization processes for medicine and dentistry practices in the developing world is a major risk factor for the propagation of disease. Modern medical facilities in the developed world often use autoclave systems to sterilize medical instruments and equipment and process waste that could contain harmful contagions. Here, we show the use of broadband light-absorbing nanoparticles as solar photothermal heaters, which generate high-temperature steam for a standalone, efficient solar autoclave useful for sanitation of instruments or materials in resource-limited, remote locations. Sterilization was verified using a standard Geobacillus stearothermophilus-based biological indicator.Item Computational chromatography: A machine learning strategy for demixing individual chemical components in complex mixtures(PNAS, 2022) Bajomo, Mary M.; Ju, Yilong; Zhou, Jingyi; Elefterescu, Simina; Farr, Corbin; Zhao, Yiping; Neumann, Oara; Nordlander, Peter; Patel, Ankit; Halas, Naomi J.; Laboratory for NanophotonicsSurface-enhanced Raman spectroscopy (SERS) holds exceptional promise as a streamlined chemical detection strategy for biological and environmental contaminants compared with current laboratory methods. Priority pollutants such as polycyclic aromatic hydrocarbons (PAHs), detectable in water and soil worldwide and known to induce multiple adverse health effects upon human exposure, are typically found in multicomponent mixtures. By combining the molecular fingerprinting capabilities of SERS with the signal separation and detection capabilities of machine learning (ML), we examine whether individual PAHs can be identified through an analysis of the SERS spectra of multicomponent PAH mixtures. We have developed an unsupervised ML method we call Characteristic Peak Extraction, a dimensionality reduction algorithm that extracts characteristic SERS peaks based on counts of detected peaks of the mixture. By analyzing the SERS spectra of two-component and four-component PAH mixtures where the concentration ratios of the various components vary, this algorithm is able to extract the spectra of each unknown component in the mixture of unknowns, which is then subsequently identified against a SERS spectral library of PAHs. Combining the molecular fingerprinting capabilities of SERS with the signal separation and detection capabilities of ML, this effort is a step toward the computational demixing of unknown chemical components occurring in complex multicomponent mixtures.Item Cooling systems and hybrid A/C systems using an electromagnetic radiation-absorbing complex(2015-05-19) Halas, Nancy J.; Nordlander, Peter; Neumann, Oara; Rice University; United States Patent and Trademark OfficeA method for powering a cooling unit. The method including applying electromagnetic (EM) radiation to a complex, where the complex absorbs the EM radiation to generate heat, transforming, using the heat generated by the complex, a fluid to vapor, and sending the vapor from the vessel to a turbine coupled to a generator by a shaft, where the vapor causes the turbine to rotate, which turns the shaft and causes the generator to generate the electric power, wherein the electric powers supplements the power needed to power the cooling unit.Item Electricity generation using electromagnetic radiation(2017-08-22) Halas, Nancy J.; Nordlander, Peter; Neumann, Oara; Rice University; United States Patent and Trademark OfficeIn general, in one aspect, the invention relates to a system to create vapor for generating electric power. The system includes a vessel comprising a fluid and a complex and a turbine. The vessel of the system is configured to concentrate EM radiation received from an EM radiation source. The vessel of the system is further configured to apply the EM radiation to the complex, where the complex absorbs the EM radiation to generate heat. The vessel of the system is also configured to transform, using the heat generated by the complex, the fluid to vapor. The vessel of the system is further configured to sending the vapor to a turbine. The turbine of the system is configured to receive, from the vessel, the vapor used to generate the electric power.Item Evolution of light-induced vapor generation at a liquid-immersed metallic nanoparticle(American Chemical Society, 2013) Fang, Zheyu; Zhen, Yu-Rong; Neumann, Oara; Polman, Albert; de Abajo, F. Javier García; Nordlander, Peter; Halas, Naomi J.; Laboratory for NanophotonicsWhen an Au nanoparticle in a liquid medium is illuminated with resonant light of sufficient intensity, a nanometer scale envelope of vapor -a “nanobubble”- surrounding the particle, is formed. This is the nanoscale onset of the well-known process of liquid boiling, occurring at a single nanoparticle nucleation site, resulting from the photothermal response of the nanoparticle. Here we examine bubble formation at an individual metallic nanoparticle in detail. Incipient nanobubble formation is observed by monitoring the plasmon resonance shift of an individual, illuminated Au nanoparticle, when its local environment changes from liquid to vapor. The temperature on the nanoparticle surface is monitored during this process, where a dramatic temperature jump is observed as the nanoscale vapor layer thermally decouples the nanoparticle from the surrounding liquid. By increasing the intensity of the incident light or decreasing the interparticle separation, we observe the formation of micron sized bubbles resulting from the coalescence of nanoparticle-“bound” vapor envelopes. These studies provide the first direct and quantitative analysis of the evolution of light-induced steam generation by nanoparticles from the nanoscale to the macroscale, a process that is of fundamental interest for a growing number of applications.Item Generating a heated fluid using an electromagnetic radiation-absorbing complex(2018-01-09) Halas, Nancy J.; Nordlander, Peter; Neumann, Oara; Rice University; United States Patent and Trademark OfficeA vessel including a concentrator configured to concentrate electromagnetic (EM) radiation received from an EM radiation source and a complex configured to absorb EM radiation to generate heat. The vessel is configured to receive a cool fluid from the cool fluid source, concentrate the EM radiation using the concentrator, apply the EM radiation to the complex, and transform, using the heat generated by the complex, the cool fluid to the heated fluid. The complex is at least one of consisting of copper nanoparticles, copper oxide nanoparticles, nanoshells, nanorods, carbon moieties, encapsulated nanoshells, encapsulated nanoparticles, and branched nanostructures. Further, the EM radiation is at least one of EM radiation in an ultraviolet region of an electromagnetic spectrum, in a visible region of the electromagnetic spectrum, and in an infrared region of the electromagnetic spectrum.Item Impurity-Induced Plasmon Damping in Individual Cobalt-Doped Hollow Au Nanoshells(American Chemical Society, 2014) Thibodeaux, Christyn A.; Kulkarni, Vikram; Chang, Wei-Shun; Neumann, Oara; Cao, Yang; Brinson, Bruce; Ayala-Orozco, Ciceron; Chen, Chih-Wei; Morosan, Emilia; Link, Stephan; Nordlander, Peter; Halas, Naomi J.; Laboratory for Nanophotonics; Rice Quantum InstituteThe optical properties of plasmonic nanoparticles in the size range corresponding to the electrostatic, or dipole, limit have the potential to reveal effects otherwise masked by phase retardation. Here we examine the optical properties of individual, sub-50 nm hollow Au nanoshells (Co-HGNS), where Co is the initial sacrificial core nanoparticle, using single particle total internal reflection scattering (TIRS) spectroscopy. The residual Co present in the metallic shell induces a substantial broadening of the homogeneous plasmon resonance line width of the Co-HGNS, where the full width at half-maximum (fwhm) broadens proportionately with increasing Co content. This doping-induced line broadening provides a strategy for controlling plasmon line width independent of nanoparticle size, and has the potential to substantially modify the relative decay channels for localized nanoparticle surface plasmons.Item Multifunctional fluorescent and MRI-active nanostructure(2022-11-22) Halas, Nancy J.; Ayala-Orozco, Ciceron; Bishnoi, Sandra; Henderson, Luke; Neumann, Oara; Pautler, Robia; Nordlander, Peter; Rice University; William Marsh Rice University; United States Patent and Trademark OfficeA Magnetic Resonance Imaging (MRI) enhancement agent includes a plurality of particles, each particle including: a metal core; a dielectric shell disposed on the metal core comprising at least one MRI contrast agent; and a metal shell disposed on the exterior surface of the dielectric shell that encapsulates the dielectric shell.Item Plasmonic Nanostructures for Solar and Biological Application(2013-09-16) Neumann, Oara; Halas, Naomi J.; Nordlander, Peter J.; Link, StephanThe electromagnetic absorption properties of plasmonic nanostructures were utilized to develop mesoscopic sites for highly efficient photothermal generation steam, SERS biosensing, and light-triggered cellular delivery uptake. Plasmonic nanostructures embedded in common thermal solutions produces vapor without the requirement of heating the fluid volume. When particles are dispersed in water at ambient temperature, energy is directed primarily to vaporization of water into steam, with a much smaller fraction resulting in heating of the fluid. Solar illuminated aqueous nanoparticle solution can drive water-ethanol distillation, yielding fractions significantly richer in ethanol content than simple thermal distillation and also produced saturated steam destroying Geobacillus stearothermophilus bacteria in a compact solar powered autoclave. Subwavelength biosensing sites were developed using the plasmonic properties of gold nanoshells to investigate the properties of aptamer (DNA) target complexes. Nanoshells are tunable core-shell nanoparticles whose resonant absorption and scattering properties are dependent on core/shell thickness ratio. Nanoshells were used to develop a label free detection method using SERS to monitor conformational change induced by aptamer target binding. The conformational changes to the aptamers induced by target binding were probed by monitoring the aptamer SERS spectra reproducibility. Furthermore, nanoshells can serve as a nonviral light-controlled delivery vector for the precise temporal and spatial control of molecular delivery in vitro. The drug delivery concept using plasmonic vectors was shown using a monolayer of ds-DNA attached to the nanoshell surface and the small molecular “parcel” intercalated inside ds-DNA loops. DAPI, a fluorescent dye, was used as the molecular parcel to visualize the release process in living cells. Upon laser illumination at the absorption resonance the nanoshell converts photon energy into heat producing a local temperature gradient that induces DNA dehybridization, releasing the intercalated molecules.Item Solar thermal desalination as a nonlinear optical process(National Academy of Sciences, 2019) Dongare, Pratiksha D.; Alabastri, Alessandro; Neumann, Oara; Nordlander, Peter; Halas, Naomi J.; Laboratory for Nanophotonics; Nanosystems Engineering Research Center for Nanotechnology-Enabled Water TreatmentThe ever-increasing global need for potable water requires practical, sustainable approaches for purifying abundant alternative sources such as seawater, high-salinity processed water, or underground reservoirs. Evaporation-based solutions are of particular interest for treating high salinity water, since conventional methods such as reverse osmosis have increasing energy requirements for higher concentrations of dissolved minerals. Demonstration of efficient water evaporation with heat localization in nanoparticle solutions under solar illumination has led to the recent rapid development of sustainable, solar-driven distillation methods. Given the amount of solar energy available per square meter at the Earth’s surface, however, it is important to utilize these incident photons as efficiently as possible to maximize clean water output. Here we show that merely focusing incident sunlight into small “hot spots” on a photothermally active desalination membrane dramatically increases––by more than 50%––the flux of distilled water. This large boost in efficiency results from the nearly exponential dependence of water vapor saturation pressure on temperature, and therefore on incident light intensity. Exploiting this inherent but previously unrecognized optical nonlinearity should enable the design of substantially higher-throughput solar thermal desalination methods. This property provides a mechanism capable of enhancing a far wider range of photothermally driven processes with supralinear intensity dependence, such as light-driven chemical reactions and separation methods.Item The Surprising in Vivo Instability of Near-IR-Absorbing Hollow Au-Ag Nanoshells(American Chemical Society, 2014) Goodman, Amanda M.; Cao, Yang; Urban, Cordula; Neumann, Oara; Ayala-Orozco, Ciceron; Knight, Mark W.; Joshi, Amit; Nordlander, Peter; Halas, Naomi J.Photothermal ablation based on resonant illumination of near-infrared-absorbing noble metal nanoparticles that have accumulated in tumors is a highly promising cancer therapy, currently in multiple clinical trials. A crucial aspect of this therapy is the nanoparticle size for optimal tumor uptake. A class of nanoparticles known as hollow Au (or Au–Ag) nanoshells (HGNS) is appealing because near-IR resonances are achievable in this system with diameters less than 100 nm. However, in this study, we report a surprising finding that in vivo HGNS are unstable, fragmenting with the Au and the remnants of the sacrificial Ag core accumulating differently in various organs. We synthesized 43, 62, and 82 nm diameter HGNS through a galvanic replacement reaction, with nanoparticles of all sizes showing virtually identical NIR resonances at ∼800 nm. A theoretical model indicated that alloying, residual Ag in the nanoparticle core, nanoparticle porosity, and surface defects all contribute to the presence of the plasmon resonance at the observed wavelength, with the major contributing factor being the residual Ag. While PEG functionalization resulted in stable nanoparticles under laser irradiation in solution, an anomalous, strongly element-specific biodistribution observed in tumor-bearing mice suggests that an avid fragmentation of all three sizes of nanoparticles occurred in vivo. Stability studies across a wide range of pH environments and in serum confirmed HGNS fragmentation. These results show that NIR resonant HGNS contain residual Ag, which does not stay contained within the HGNS in vivo. This demonstrates the importance of tracking both materials of a galvanic replacement nanoparticle in biodistribution studies and of performing thorough nanoparticle stability studies prior to any intended in vivo trial application.Item Waste remediation(2017-01-17) Halas, Nancy J.; Nordlander, Peter; Neumann, Oara; Rice University; United States Patent and Trademark OfficeA system including a steam generation system and a chamber. The steam generation system includes a complex and the steam generation system is configured to receive water, concentrate electromagnetic (EM) radiation received from an EM radiation source, apply the EM radiation to the complex, where the complex absorbs the EM radiation to generate heat, and transform, using the heat generated by the complex, the water to steam. The chamber is configured to receive the steam and an object, wherein the object is of medical waste, medical equipment, fabric, and fecal matter.Item Waste remediation(2015-12-29) Halas, Nancy J.; Nordlander, Peter; Neumann, Oara; Rice University; United States Patent and Trademark OfficeA system including a steam generation system and a chamber. The steam generation system includes a complex and the steam generation system is configured to receive water, concentrate electromagnetic (EM) radiation received from an EM radiation source, apply the EM radiation to the complex, where the complex absorbs the EM radiation to generate heat, and transform, using the heat generated by the complex, the water to steam. The chamber is configured to receive the steam and an object, wherein the object is of medical waste, medical equipment, fabric, and fecal matter.