Highly sensitive detection of low abundant molecules by pyro-electrohydro-dynamic jetting

The effective detection of low-concentrated molecules in small volumes represents a significant challenge in many sectors such as biomedicine, safety, and pollution. Here, we show an easy way to dispense liquid droplets from few μl volume (0.2-0.5 μl) of a mother drop, used as reservoir, by using a pyro-electrohydro-dynamic jetting (p-jet) dispenser. This system is proposed for multi-purpose applications such as printing viscous fluids and as a biosensor system. The p-jet system is based on the pyroelectric effect of polar dielectric crystals such as lithium niobate (LN). The electric field generated by the pyroelectric effect acts electro-hydrodynamically on the sample of liquid, allowing the deposition of small volumes. The p-jet approach allows to obtain the dispensing of drops of very small volumes (up to tenths of a picoliter) avoiding the use of syringes and nozzles generally used in standard technologies. The reliability of the technique as a biosensor is demonstrated both in the case of oligonucleotides and in a sample of clinical interest, namely gliadin. The results show the possibility of detecting these biomolecules even when they are low abundant, i.e. down to attomolar. The results show a marked improvement in the detection limit (LOD) when compared with the conventional technique (ELISA). Moreover, it has been presented the possibility of using the p-jet as a useful tool in the detection of biomarkers, present in the blood but currently not detectable with conventional techniques and related to neurodegenerative diseases such as Alzheimer.

[1]  P. Ferraro,et al.  Pyro-electrification of polymer membranes for cell patterning , 2016 .

[2]  P. Ferraro,et al.  Pyro-Electrification of Freestanding Polymer Sheets: A New Tool for Cation-Free Manipulation of Cell Adhesion in vitro , 2019, Front. Chem..

[3]  A. Roda,et al.  Recent advancements in chemical luminescence-based lab-on-chip and microfluidic platforms for bioanalysis. , 2014, Journal of pharmaceutical and biomedical analysis.

[4]  Chen Zhu,et al.  Flexible small-channel thin-film transistors by electrohydrodynamic lithography. , 2017, Nanoscale.

[5]  Vittorio Bianco,et al.  Detection of self-propelling bacteria by speckle correlation assessment and applications to food industry , 2019, Optical Metrology.

[6]  P. Ferraro,et al.  Twice electric field poling for engineering multiperiodic Hex-PPLN microstructures , 2017 .

[7]  Moonsub Shim,et al.  Direct laser writing of air-stable p-n junctions in graphene. , 2014, ACS nano.

[8]  Chuan Zhao,et al.  Robust and versatile ionic liquid microarrays achieved by microcontact printing , 2014, Nature Communications.

[9]  P. Ferraro,et al.  Easy Printing of High Viscous Microdots by Spontaneous Breakup of Thin Fibers. , 2018, ACS applied materials & interfaces.

[10]  Pietro Ferraro,et al.  Simple and Rapid Bioink Jet Printing for Multiscale Cell Adhesion Islands. , 2017, Macromolecular bioscience.

[11]  Geoffrey Ingram Taylor,et al.  Disintegration of water drops in an electric field , 1964, Proceedings of the Royal Society of London. Series A. Mathematical and Physical Sciences.

[12]  P. Maddalena,et al.  Direct Evidence of Polar Ordering and Investigation on Cytophilic Properties of Pyroelectrified Polymer Films by Optical Second Harmonic Generation Analysis , 2017 .

[13]  V Marchesano,et al.  Pyroelectric Effect Enables Simple and Rapid Evaluation of Biofilm Formation. , 2018, ACS applied materials & interfaces.

[14]  John A Rogers,et al.  Functional protein microarrays by electrohydrodynamic jet printing. , 2012, Analytical chemistry.

[15]  Pietro Ferraro,et al.  Investigation on cone jetting regimes of liquid droplets subjected to pyroelectric fields induced by laser blasts , 2015 .

[16]  Pietro Ferraro,et al.  Bipolar Patterning of Polymer Membranes by Pyroelectrification. , 2016, Advanced materials.

[17]  C. Nylander,et al.  Chemical and biological sensors , 1985 .

[18]  P. Ferraro,et al.  A skin-over-liquid platform with compliant microbumps actuated by pyro-EHD pressure , 2019, NPG Asia Materials.

[19]  P. Ferraro,et al.  Maskless Arrayed Nanofiber Mats by Bipolar Pyroelectrospinning. , 2019, ACS applied materials & interfaces.

[20]  Romina Rega,et al.  Spiral formation at microscale by μ-pyro-electrospinning , 2016 .

[21]  Rustem F Ismagilov,et al.  A droplet-based, composite PDMS/glass capillary microfluidic system for evaluating protein crystallization conditions by microbatch and vapor-diffusion methods with on-chip X-ray diffraction. , 2004, Angewandte Chemie.

[22]  L Battista,et al.  Active accumulation of very diluted biomolecules by nano-dispensing for easy detection below the femtomolar range , 2014, Nature Communications.

[23]  J. R. Melcher,et al.  Electrohydrodynamics: A Review of the Role of Interfacial Shear Stresses , 1969 .

[24]  Stéphane Popinet,et al.  A charge-conservative approach for simulating electrohydrodynamic two-phase flows using volume-of-fluid , 2011, J. Comput. Phys..

[25]  Jennifer N Cha,et al.  Large-area spatially ordered arrays of gold nanoparticles directed by lithographically confined DNA origami. , 2010, Nature nanotechnology.

[26]  R. Rega,et al.  A pyroelectric-based system for sensing low abundant lactose molecules , 2019, Optical Metrology.

[27]  Vittorio Bianco,et al.  Biospeckle Decorrelation Quantifies the Performance of Alginate-Encapsulated Probiotic Bacteria , 2019, IEEE Journal of Selected Topics in Quantum Electronics.

[28]  J. Hardy,et al.  Alzheimer's disease: the amyloid cascade hypothesis: an update and reappraisal. , 2006, Journal of Alzheimer's disease : JAD.

[29]  E. Kumacheva,et al.  Patterning surfaces with functional polymers. , 2008, Nature materials.

[30]  Jun Yeob Song,et al.  High‐Resolution Printing of 3D Structures Using an Electrohydrodynamic Inkjet with Multiple Functional Inks , 2015, Advanced materials.

[31]  John Zeleny,et al.  Instability of Electrified Liquid Surfaces , 1917 .

[32]  A. Irace,et al.  Investigation of pyroelectric fields generated by lithium niobate crystals through integrated microheaters , 2017 .

[33]  Bert Popping,et al.  Comparative study of commercially available gluten ELISA kits using an incurred reference material , 2013 .

[34]  B. Ju,et al.  Flexible Plasmonic Color Filters Fabricated via Nanotransfer Printing with Nanoimprint-Based Planarization. , 2017, ACS applied materials & interfaces.

[35]  Sunny,et al.  Sol-gel assisted nano-structured SnO2 sensor for low concentration ammonia detection at room temperature , 2019, Materials Research Express.

[36]  M Paturzo,et al.  Dispensing nano-pico droplets and liquid patterning by pyroelectrodynamic shooting. , 2010, Nature nanotechnology.

[37]  Y. Rim,et al.  Recent Progress in Materials and Devices toward Printable and Flexible Sensors , 2016, Advanced materials.