Aqueous Solutions and other Polar Liquids Perturbed by Serial Dilutions and Vigorous Shaking: Analyses of Their UV Spectra

In summary, the basic tenets of the QED SDVSPL model are: For solutions of polar liquids, there exist solute type dependent transition concentrations at which specific QED domains may become stabilized; solutes’ characteristics determine the stabilization of the domains; once domains of type CD_rot and CD_elec become stabilized, serial dilutions in combination with vigorous shaking cause the perpetuation of these domains in the resulting dilutes. In other words, after at C< the domain of type CD_rot forms, the solutes are not any longer needed for stabilizing additional CD_rot and CD_elec in the dilutes.

The QED model of SDVSPL is congruent with recently empirically-based models. The main aspects of the model of Konovalov and Ryzhkina (2014, 2016), which they based on their extensive experimental data, are as follows: During the SDVSPL preparation procedure, for many but not all kinds of solutes, for C less than a solute type dependent C_thr, nano-sized self-organized substrate-induced molecular ensembles (associates) stabilize. The term “substrate” refers to the solute in the stock (mother) solution from which the SDVSPL is prepared. The characteristics of the associates are such that these constitute a phase which is different from the medium, i.e., SDVSPL are nano-heterogeneous. Consequently, these SDVSPL cannot strictly be regarded as solutions in the customary sense. Instead, these are nano-disperse systems. Nano-sized associates composed of polar liquid molecules (the original solvent molecules) constitute the disperse phase. For SDVSPL with C above the Avogadro limit, the experimental data is yet insufficient for determining the distribution of the solute molecules located in the associates versus those located in the dispersion medium (the polar liquid). While SDVSPL are highly diluted, the substrate’s content decreases. Yet, nano-sized associates, solely composed of the polar liquid’s (original solvent) molecules, persist. Thus, on serial diluting a polar liquid’s solution, in combination with vigorous shaking the liquid after each dilution step, a special kind of disperse system emerges — a disperse system of polar liquid associates immerged in a polar liquid (the medium). The electronic structure and the ordering of the polar liquid molecules in the associates are determined by the characteristics of the substrate molecules. Therefore, the associates contain the molecular information of the substrate. However, the specific relation between the characteristics of the substrate and the electronic state and molecular ordering of the associates has not yet been discovered.

The model proposed by Elia et al.  (2014, 2015), which is based on their extensive experimental data, also emphasizes the aggregates (molecular ensembles) composed of the polar liquid (solvent) molecules in SDVSPL, described in the previous paragraph. In addition, their model addresses the solid phase which is obtainable by isolating the aggregates. The aggregates can be “extracted” by evaporating SDVSPL in air at ambient temperatures, by evaporation at high temperatures (90^o C) or by lyophilizing. The solid, i.e., the isolated aggregates, is soluble in the polar liquid. After dissolving the solid in the pure polar liquid, the liquid’s physicochemical parameters are almost exactly like those of the original SDVSPL from which the solid was extracted. As such the model emphasizes that the aggregates are a phase which differs from the known liquid and ice phases of polar
liquids.

^c I thank the anonymous reviewer for bringing to my attention the paper by Elton and Fernandez-Serra (Nature Communications 2016). Its analyses reveal a property of water conforming to an aspect of the dynamics of H₂O constituting CD_rot . Its analyses of Raman and infrared spectroscopic data indicate the presence of coherent long-range dipole–dipole interactions in water. As to additional experimental evidence for properties of CD_rot, analyses of dielectric permittivity measurements of SDVSPL have shed light on their ferroelectric properties (Yinnon and Liu, 2016). Moreover, analyses of thermogravimetric measurements of water perturbed by a Nafion membrane have provided information on the transition concentration below which these domains can become stabilized adjacent to the membrane (Yinnon et al., 2016).

Analyses of Published Experimental Data on UV Radiation’s Absorbance, Fluorescence and Transmission

Aqueous SDVSPL, prepared in glass containers, absorb radiation in the 190 – 325 nm range (Lo 1996; Lobyshev et al., 2005; Wolf et al., 2011; Klein et al., 2013; Ghosh et al. 2015; Elia et al., 2014; Chakraborty et al., 2015). The UV radiation’s absorbance, transmission or fluorescence by aqueous SDVSPL prepared in plastic containers, to the best of our knowledge, has not been reported.

The absorbance spectra of aqueous SDVSPL mainly are typified by three broad absorbance bands (Lo 1996; Lobyshev et al., 2005; Ghosh et al. 2015; Elia et al., 2014; Chakraborty et al., 2015). The wavelengths of the bands’ maxima are in the range of 205 – 210 nm, 260 – 280 nm and 300 – 310 nm. The wavelengths of the maxima slightly non-monotonically depend on the number of dilution steps. The half-widths of the bands are about 20 – 30 nm.

UV-vis radiation fluorescence features of SDVSPL have been reported for aqueous SDVSPL of NaCl and for SDVSPL-of-Distilled-Water (Lobyshev et al., 2005).^d These SDVSPL were irradiated with 300 nm radiation. The fluorescence spectra consist of a broad band with maximum at about 385 nm. The half-width of the band is about 100 nm. For SDVSPL-of-Distilled-Water, the fluorescence intensity non-monotonically changes with the number of dilution step (NDS). For aqueous SDVSPL of NaCl, at concentrations below C≈10^-7 M≈C_thr,^e the fluorescence intensity also non-monotonically changes with NDS. For both these SDVSPL, the intensity non-monotonically varies with the storage time of the samples. The samples were stored in glass bottles closed with lids. The samples were stored in the dark at room temperature.

The transmission of UV radiation by aqueous SDVSPL of NaCl, aqueous SDVSPL of nitric acid (HNO₃) and aqueous SDVSPL of sodium hydroxide (NaOH) has been measured by Lo (1996). These SDVSPL were decimally diluted and had concentrations in the range of 10^-3 M to 10^-13 M. On decreasing the concentration of these SDVSPL from 10^-3 M to10^-5 M, the transmission increased. However, for concentrations below about 10^-5 – 10^-7 M, the transmission non-monotonically changed with NDS.

Highly controlled, blinded and randomized experiments of UV radiation transmission by SDVSPL were carried out by Wolf et al. (2011) and Klein et al. (2013). They measured the transmission of UV radiation by aqueous SDVSPL of copper sulfate (CuSO₄), aqueous SDVSPL of hypericum and aqueous SDVSPL of sublimed sulfur (S₈). These SDVSPL were 6 to 30 times centesimally or decimally diluted. Statistical analyses of the data show that the UV radiation’s transmission of these aqueous SDVSPL significantly differ from that of the controls. The controls were vigorously shaken solvents. These solvents were of the various types of purified waters or the 99% water and 1% ethanol mixture with which the SDVSPL were prepared. The purified waters included distilled water, Quartz distilled water and de-ionized water. Some of the experiments were carried out in a metal-free class 100 High Efficiency Particulate Air (HEPA) filtered clean room. Clean flow boxes had class 5. These experiments showed that the UV radiation’s transmission by aqueous SDVSPL of CuSO₄ or aqueous SDVSPL of hypericum is lower than that of the control. However, for aqueous SDVSPL of S₈, it is higher than the control.

Transmission of UV radiation measurements also showed that the properties of the residues of evaporated SDVSPL depend on the NDS and the solute used in their preparation (Klein and Wolf, 2016). SDVSPL were poured on sugar globules. The solvent in these SDVSPL was ethanol.

The globules were left to dry in air. Subsequently, the globules together with their residue of the evaporated SDVSPL were dissolved in water. The resultant liquid’s UV radiation’s transmission was measured. For SDVSPL of Aconitum napellus, Atropa belladonna, phosphorus, sulfur, Apis mellifica, quartz, which were 30 and 200 times centesimal diluted, the transmissions statistically significant differed.

^d SDVSPL-of-Distilled-Water is prepared by serially diluting distilled water and vigorously shaken the liquid after each dilution step.

^e C_thr of aqueous SDVSPL of NaCl have been measured by Ryzhkina et al. (2012c).

Analyses of UV Radiation Absorbance

The UV radiation’s absorbance by all aqueous SDVSPL, including those diluted much below the Avogadro limit, significantly differs from that of pure non-serially diluted non-vigorously shaken water in its various phases, e.g., bulk water, gas phase water, amorphous-, hexagonal- or cubic-ice. A UV absorbance band with a maximum around 270 nm, which exists in the UV spectra of SDVSPL, was also observed in water by Larzul et al. in 1965. However, subsequent extensive research has shown that pure water does not absorb in this range (Quickenden and Irvin, 1980; Mulliken and Ermler, 1981; Segarra-Martí, 2013). Hence, the absorbance band around 270 nm measured by Larzul et al. (1965) had been attributed to impurities. For gas phase H₂O, its lowest-energy band of the electronic spectrum covers the 151 – 182 nm range with a maximum at 168 nm. In pure bulk liquid water, this band is broader and blue-shifted. Its maximum is at 151 nm and its absorbance falls off monotonically by about ten orders of magnitude in the 151 – 400 nm range (it is only about 0.0001 cm^-1 at 320 nm). Amorphous, hexagonal or cubic ice has absorbance features similar to those detailed in the previous sentence (Quickenden and Irvin, 1980; Cabral do Couto et al., 2012; Segarra-Martí et al., 2013).

The UV radiation’s absorbance features of aqueous SDVSPL resemble those of structured waters. For example, a UV absorbance band in the 225 – 325 nm range, with a maximum around 260 – 280 nm, is typical for structured waters (Segarra-Martí et al., 2013). Such a band has been observed for example for the following waters:

• the ordered water adjacent to hydrophilic membranes like Nafion [so called exclusion zone (EZ) water] (Zeng et al., 2006);
• water perturbed with a Nafion membrane (Elia et al., 2013b, 2014b);
• water perturbed with cellulose (Elia et al., 2018);
• water-ethanol mixtures (Liu et al., 2007);
• iterative filtered water (Elia et al., 2014c);
• aqueous solutions of non-luminescence compounds (e.g. aqueous glycylasparagine at 10^-9 M<C<10^-3 M, aqueous alkali chlorides at ~1 M< C< ~ 5 M, aqueous L-lysine monohydrochloride at 0.1 M< C<1 M, D-alanine, or aqueous D-glucose at 0.1 M< C<1 M) (Lobyshev et al., 1999; Chai et al., 2008).

As to the absorbance band with maxima in the range of 205 – 210 nm observed for aqueous SDVSPL, such a band has also been measured for the following structured waters: for EZ water (Zheng et al., 2006), for water perturbed with a Nafion membrane (Elia et al., 2013a) and for water perturbed with cellulose (Elia et al., 2018). A similar band has been observed for magnetized water (Pang, 2014).

The resemblances between the UV radiation’s absorbance features of aqueous SDVSPL and those of the above listed structured waters suggest that some information on the structuring of H₂O in the former can be obtained from analyses of the latter. From the above list of structured waters, that of water perturbed with a Nafion membrane has recently been extensively analyzed with many state-of-the-art techniques (Elia et al., 2013a, 2013b, 2014c, 2015, 2017; Capolupo et al., 2014; Yinnon et al., 2016). The analyses show that its UV absorbance and fluorescence is due to its H₂O aggregates. It contains 10^-4 mol / liter of micron-sized H₂O aggregates. Its chemical analyses showed that it contains 10^-6 mol / liter non-H₂O compounds, i.e., fluorine (F^–) and sulfate (HSO₄^–) ions released by the Nafion membrane. The very low concentration of these non-H₂O compounds implies that these cannot underlie formation of the H₂O aggregates or the significant UV absorbance. Instead, the various analyses of the data obtained for water perturbed by a Nafion membrane indicate that its aggregates are composed of  and CD_rot (Capolupo et al., 2014; Elia et al, 2015, 2017; Yinnon et al., 2016). The analyses also indicate that this water’s UV radiation’s absorbance features can be attributed to . Also the more restricted analyses of the H₂O aggregates constituting EZ water, the molecular associates in aqueous solutions and the aggregates in water perturbed with cellulose indicate that these include  (Del Giudice et al., 2013; Yinnon and Yinnon, 2009; Yinnon et al., 2016; Elia et al., 2018). Accordingly, because of the resemblance of the UV radiation’s absorbance features of aqueous SDVSPL and water perturbed with a Nafion membrane or cellulose, EZ water and aqueous solutions, also for aqueous SDVSPL these features are attributable to . Indeed the QED of SDVSPL model and the analyses of many other measured physicochemical properties of aqueous SDVSPL indicate that these liquids contain  (see paragraphs I, II, IV and V, and Yinnon and Liu, 2015b&c). The analyses of the UV-vis radiation’s fluorescence of aqueous SDVSPL, presented in the next sub-section, provide additional evidence that  underlie the UV radiation’s absorbance features.

Analyses of UV-vis Fluorescence

The above-cited fluorescence features of aqueous SDVSPL resemble those of the structured waters listed in the previous sub-section, i.e., when these structured waters were excited with radiation with wavelengths in the 225 – 325 nm range. The fluorescence spectra of all these waters consist of a rather featureless broad band (Lobyshev et al., 1999, 2005; Liu et al., 2007; Chai et al., 2008; Elia et al., 2017). The wavelengths of the band and of its maximum depend on the method with which the water was perturbed. It also depends on the type of solutes. Moreover, for aqueous solutions of glycylasparagine, Lobyshev et al. (1999) showed that that just as for aqueous SDVSPL, their fluorescence intensity may increase during their storage in a dark place.

The absence of any sharp peaks in the fluorescence spectra of the above listed structured waters indicates that excimers are present^f (Liu et al., 2007, 2012; Segarra-Martí et al., 2013, 2014). In particular, the excimers underlying the structure of EZ water have been in depth analyzed. The analyses have been carried out with high-level computations, i.e., with the well established quantum mechanical ab initio derived Complete-Active-Space Self-Consistent-Field second-order perturbation theory (CASPT2) (Segarra-Martí et al., 2013, 2014). The analyses indicate the following: EZ waters contain aggregates which are composed of excimers forming networks of multilayer honeycomb ice-like layers (see Fig. 1 and 6 in Segarra-Martí et al., 2014). The formula of the excimers is H₃₈O₂₀. The formula of the two monomers constituting the excimer is H₁₉O₁₀. The H₂O forming the monomer are organized in two fused hexagons. The electronic properties of the H₃₈O₂₀ excimer is a function of its inter-monomer distance, i.e., its structural relaxation.

The quantum mechanics excimer-based model of EZ water has important features in common with the quantum dynamic QED model of EZ water developed by Del Giudice et al. (2013). Elia et al. (2017) first pointed out the similarities between these models. In the H₃₈O₂₀ excimer, each of the two central (fused) H₂O of one monomer attracts its opposite central (fused) H₂O of the other monomer (See Fig. 6 in Segarra-Martí et al., 2014). The attractive interaction is due to π-stacking. In the H₃₈O₂₀ networks, the π-stacked H₂O resonate between their ground and an excited electronic state, i.e., about 10 percent of the H₂O constituting the network are simultaneously electronically excited.  According to QED, in a , the H₂O also resonate between their ground and an excited electronic state. About 10 percent of the H₂O constituting the are simultaneously electronically excited. One of the differences between the excimer and QED models is that the former predicts that the π-stacked H₂O resonate between two of their electronic states, while the latter predicts that all of the about 10⁶ H₂O composing a resonate between two of their electronic states. For many body condensed systems, quantum electro-dynamics is a more accurate theory than quantum mechanics (Preparata, 1995).

Analyses of experimental data have indicated that aggregates with properties of  or of excimers are present in the following structured waters: in non-vigorously shaken aqueous solutions of alkali halides or glucose with C in the 1 – 10^-3 M range, water-alcohol mixtures, aqueous deoxyribonucleic acid (DNA) with C in the range 2.5 – 0.25 g dL^-1 (Liu et al., 2007; Yinnon and Yinnon, 2009; Segarra-Martí et al., 2013); in EZ water (Del Giudice et al., 2013; Segarra-Martí et al., 2013, 2014; Yinnon et al., 2016); and in water perturbed with a Nafion membrane or cellulose (Elia et al., 2015, 2017; Yinnon et al., 2016). Hence, the UV-vis fluorescence of structured waters is attributable to associates of water molecules, wherein part of the H₂O transit between their ground and an excited electronic state, i.e., aggregates composed of excimers or their quantum dynamics analogous QED .

The resemblance between the UV-vis fluorescence features of aqueous SDVSPL and those of the above cited structured waters evokes that the fluorescence of aqueous SDVSPL also is due to . Or alternatively, these features may be due to the quantum mechanic aggregates composed of excimers. To corroborate this evocation, in the next two sub-sections are represented, respectively, for aqueous SDVSPL of NaCl and SDVSPL-of-Distilled-Water, the fine-details of their fluorescence after their irradiation with 300 nm radiation. Subsequently, the details are analyzed within the context of QED.

f The characteristics of excimers, the mechanisms underlying their formation and their UV-vis emission features are summarized in the Appendix of the paper by Elia et al. (2017).

Details of the UV-vis Fluorescence Features of SDVSPL of NaCl and Their Explanation

The details, which are summarized in Fig. 1 and in the table in Lobyshev et al. (2005) are:

• The fluorescence intensity of samples with C=2 M, one day after their preparation, is about seven times larger than that of distilled water. For 2×10^-3 M<C <2 M, the fluorescence intensity monotonically drops by about a factor of five. For C<2×10^-3 M, the fluorescence intensity non-monotonically changes with C. For C in the range of 2×10^-4 M – 2×10^-24 M, the values of the intensity vary between that of distilled water and values twice or even four times larger than that of distilled water. Pronounced maxima in the intensity are observed for C = 2×10^-1 M, C = 2×10^-8 M, C=2×10^-12 M, C=2×10^-19 M and for a 28 times decimal diluted solution. The strongest maxima are the ones at C = 2×10^-1 M and C=2×10^-12 M. Both maxima are about 250 percent higher than the other maxima.
• The fluorescence intensity non-monotonically varies with the storage time of the samples. During the six weeks after their preparation, the intensity may decrease or increase by as much as 50 – 80 percent.
• The fluorescence intensity is negatively correlated with the motility of the infusorium Spirostoma ambiguum in the SDVSPL.

Explanations for the above presented UV-vis fluorescence features of aqueous SDVSPL of NaCl are feasible within the context of the results of the extensive studies of aqueous NaCl and of aqueous SDVSPL of NaCl which were carried out during the last two decades. In the following, I cite the relevant data and with the QED model of SDVSPL I explain the UV-vis fluorescence features of aqueous SDVSPL of NaCl obtained by Lobyshev et al. (2005).

◉ For 0.68 M< C< 5.32 M, in non-vigorously shaken aqueous NaCl, dynamic light scattering (DLS) revealed the presence of domains with diameters in the 10² – 10³ nm range and small clusters with sizes of 0.1 – 0.4 nm (Georgalis et al., 2000; Samal and Geckeler, 2001; Sedlak 2006). The clusters are hydrated ions. The domains are not nano-bubbles (Sedlak and Rak, 2013). In aqueous SDVSPL of NaCl, for 0.15 M<C<1.8 M, DLS also revealed hydrated ions and 10² – 10³ nm sized domains (Ryzhkina et al., 2012c). For C<0.15 M, DLS cannot clearly distinguish domains, except for ~220 nm sized domains at C=2×10^-10 M (Ryzhkina et al., 2012c). Yet, also for C<0.15 M, electrical conductivity and UV absorbance measurements have indicated that molecular associates are present in these solutions (Lo, 1996, 2013; Lo et al., 2009; Elia and Niccoli, 2004a; Ryzhkina et al., 2012c).

Analyses of the characteristics of the domains and their impact on the physicochemical properties of the solutions, for C>0.15 M, showed that the domains include the 10³ nm sized CD_plasma and supra-CD_plasma, which stabilized the 10² nm sized  and supra- (Yinnon and Yinnon, 2009, 2012; Yinnon and Liu, 2015b). As such the analyses confirmed the characteristic of the QED model of SDVSPL detailed in paragraph I.

The presence of  with their pool of quasi free electrons (QFE) in aqueous NaCl solutions at the aforementioned concentrations (or their analogous quantum mechanics agglomerates composed of excimers), explain the strong UV absorbance and fluorescence of these solutions observed by Lobyshev et al. (2005). In other words, just as for EZ water or water perturbed with a Nafion membrane or with cellulose, for which similar UV phenomena were observed and shown to be attributable to  or excimers (Chai et al., 2008; Elia et al., 2013a, 2017, 2018; Yinnon et al., 2016), also the UV phenomena of aqueous NaCl are attributable to . As to the decrease in the fluorescence observed on dilution from C=2 M to C=2×10^-3 M, it is attributable to the diminishment of the number of solutes affecting CD_plasma and thus reducing the stabilization of .

◉ On reducing C form ~10^-3 M to ~10^-6 M, for aqueous SDVSPL of NaCl, Lo (1996) observed a fall off in the UV absorbance in the190 – 250 nm range, while Ryzhkina et al. (2012c) observed a fall off in χ. The fall offs were shown to be ascribable to the reduction in the number of IPD_plasma and EDA^IPDplasma, which caused a diminishment in the number of stabilized  (Yinnon and Liu, 2015b). The diminishment explains the fall offs in the UV fluorescence intensity observed by Lobyshev et al. (2005).

◉ At C< ~10^-6 M, for aqueous SDVSPL of NaCl, their observed physicochemical variables (e.g., dielectric constant, UV absorbance in the190 -250 nm range, χ, heat of mixing and pH), all non-monotonically vary with the number of dilution steps (Lo, 1996; Lo et al., 1996; Elia and Niccoli, 2004a; Ryzhkina et al., 2012c). QED analyses have shown that the non-monotonic variation is attributable to the realignments of CD_rot. For C below the critical concentration , CD_rot become stabilized by EDA^IPDplasma (Yinnon and Yinnon, 2011; Yinnon and Elia, 2013; Yinnon and Liu, 2015b&c). For aqueous SDVSPL of NaCl,  is about 10^-7 M (Yinnon and Liu, 2015b). In addition, the QED analyses have indicated that the vigorous shaking of the SDVSPL after each dilutions step breaks up the CD_rot. Due to the ferroelectric ordering of the H₂O constituting the CD_rot, these domains’ broken pieces also have a net electric dipole moment, i.e., these are the electric dipole aggregates EDA^CDrot. These aggregates stabilize new CD_rot. The dilution, shaking and resulting break up of CD_rot cause realignments of these domains’ electric dipole moments, i.e., affect the polarization of the liquid.

QED analyses of experimental data on aqueous SDVSPL have indicated that CD_rot may stabilize  (Yinnon and Liu, 2015c). The stabilization is influenced by the polarization of the liquid. Since after each dilution and vigorous shaking step, the polarization changes, the prevalence of  non-monotonically varies with the number of dilutions steps.

Based on the findings of the QED analyses pointed out above, it is possible to account for the non-monotonic dependence on the number of dilution steps of the fluorescence of aqueous SDVSPL of NaCl for C< ~10^-6 M, observed by Lobyshev et al. (2005). The variation is attributable to the non-monotonic dependence on the number of dilution steps of the prevalence of  stabilized by CD_rot in this concentration range.

◉ A high maximum in the fluorescence intensity of aqueous SDVSPL of NaCl for C< , i.e., the one at C=2×10^-12 M, is a feature which also has been observed for other physicochemical variables of SDVSPL (Miranda et al., 2011; Ryzhkina et al., 2012c; Nain et al., 2015). However, the number of dilutions steps at which the maximum appeared is not the same for SDVSPL investigated by independent research groups. It should be stressed that even just the distilled water with which the SDVSPL are produced affects the maximum — distilled waters produced in different companies affect the maximum in different ways. The hysteretic and far-our-of-equilibrium properties of SDVSPL explain the variance of the concentration at which the maximum appears. These properties imply that each experimental set up greatly affects the alignment of CD_rot and hence the prevalence of .

It should be emphasized that the prevalence of  is not solely affected by the alignment of CD_rot. In the presence of ions, external alternating magnetic fields may enhance the stabilization of  (Del Giudice et al., 2002; Yinnon, 2017). For example, the ambient Schumann resonances may enhance the stabilization. The effect of the alternating magnetic field depends on the concentration and other characteristics of the ions (Montagnier et al., 2011, 2015). Hence, maxima in the prevalence of  should depend also on the concentration of the SDVSPL and the characteristics of its original solute.

◉ The storage time dependence of the non-monotonic variation of the fluorescence intensity of aqueous SDVSPL of NaCl, observed by Lobyshev et al. (2005), is a phenomenon these liquids have in common with other measured physicochemical variables of numerous types of SDVSPL and other structured waters (Elia et al., 2004a, 2005, 2008a&b; Belon et al., 2008, Elia et al., 2013b, 2015). QED analyses showed that the variation is due to these liquids residing in a far-out-of-equilibrium state (Yinnon and Elia, 2013; Yinnon et al., 2016). CD_rot continuously realign, agglomerate into supra- CD_rot and alter the stabilization of and supra-. The peculiar quasi-periodic dynamics of these domains have been analyzed by Yinnon and Elia (2013).

◉ The fluorescence intensity of the SDVSPL of NaCl, which is negatively correlated with the motility activity of the infusorium Spirostoma ambiguum in this media (Lobyshev et al., 2005)  is yet another example of the relation between the physicochemical properties of numerous SDVSPL and their bio-activity (Konovalov and Ryzhkina, 2014). Elucidating the effects of SDVSPL on biosystems is hampered by the many unsolved puzzles pertaining to biochemical reactions. Yet the discussion by Yinnon and Liu (2015c) and Yinnon (2017) hints that  play a role. The observed relation between the fluorescence intensity and the motility activity therefore is not surprising.

SDVSPL-of-Distilled-Water Samples’ UV-vis Fluorescence Features and Their Explanations

In order to differentiate between the impact of the solute (NaCl) on the properties of the fluorescence of aqueous SDVSPL of NaCl, as well as the impact of the serial dilutions and vigorous shaking, Lobyshev et al. (2005) also measured the fluorescence of SDVSPL-of-Distilled-Water. On irradiating such perturbed water samples with 300 nm radiation, they mainly observed the following fluorescence spectral features [see Fig. 2 in Lobyshev et al. (2005)]:

★ The spectra are similar to those of aqueous SDVSPL of NaCl.

★ For SDVSPL-of-Distilled-Water which was 1 to 12 times decimally diluted, the luminescence intensity is about three to five times larger than that of “normal” distilled water. Here “normal” distilled water refers to water which was not vigorously shaken and not serially diluted.

★ For SDVSPL-of-Distilled-Water which was 13 to 30 times decimal diluted, the fluorescence intensity values vary between that of “normal” distilled water or are about twice as high.

★ The fluorescence intensities of SDVSPL-of-Distilled-Water, just as for aqueous SDVSPL of NaCl, non-monotonically depend on the time of its storage.

Explanations for these spectral features are feasible within the context of the findings of the extensive studies of SDVSPL-of-Distilled-Water or SDVSPL-of-ethanol. These studies were carried out by independent researchers during the last decade (Elia and Niccoli, 2004a, 2005; Miranda et al, 2011; Upadhyay and Nayak, 2011; Nain et al., 2015). These studies have shown that the values of the physicochemical variables (e.g., χ, Q, pH, viscosities, densities, ultrasonic speeds or refraction index) of SDVSPL-of-Distilled-Water or SDVSPL-of-ethanol significantly differ, respectively, from those of “normal” distilled water or “normal” ethanol.

The differences between SDVSPL-of-Distilled-Water and “normal” distilled water are not directly attributable to compounds released by the glass container or other impurities, as evidenced by the carefully controlled experiments carried out by Elia and Niccoli (2004a, 2005). They showed that the vigorous shaking indeed released compounds from the glass, e.g., Na⁺ or SiO₂. They showed that the concentration of these compounds in SDVSPL-of-Distilled-Water was of the order of 10^-5 M or below. However, these compounds could not account for the physicochemical properties of the SDVSPL-of-Distilled-Water. They showed that for the control, i.e., “normal” distilled water with the same chemical composition as SDVSPL-of-Distilled-Water, the values of its physicochemical variables significantly differ from those of SDVSPL-of-Distilled-Water. Here “normal” distilled water “with the same chemical composition as SDVSPL-of-Distilled-Water” refers to “normal” distilled water containing the same compounds released by the glass, which are present at the same concentrations.

Elia and Niccoli (2004a, 2005) showed that vigorous shaking of the SDVSPL-of-Distilled-Water altered the ordering of its H₂O. They showed that on omitting the vigorous shaking, the physicochemical variables of serial diluted liquids and “normal” liquids were the same. They also showed that the SDVSPL-of-Distilled-Water is a far-out-of equilibrium system. Changes in its H₂O orderings continuously occur for many months after its preparation. They observed that on aging of the liquid, the electric conductivity, heat of mixing and pH values vary non-monotonically (Elia et al., 2000, 2008a&b; Belon et al., 2008).

In regard of the findings by Elia and Niccoli (2004a, 2005, 2008a&b) and those of the other groups which investigated SDVSPL-of-Distilled-Water, it is not surprising that the UV-vis fluorescence features of SDVSPL-of-Distilled-Water observed by Lobyshev et al. (2005) also differ from those of “normal” distilled water. Moreover, it is not surprising that the fluorescence intensity of SDVSPL-of-Distilled-Water varied non-monotonically with the storage time of these liquids.

Based on the experimental data and theoretical developments that accumulated during the last decade, the following two complementary mechanisms can explain the differences between the ordering of the solvent molecules in SDVSPL-of-polar liquids and “normal” polar liquids.

A. “Activation” of the ordering of the H₂O in SDVSPL-of-Distilled-Water by compounds released by the glass containers has been conjectured by Elia and Niccoli (2004a). It should be emphasized that Elia and Niccoli (2004a) conjectured that the changes are activated by the compounds, but not simply due to the presence of the compounds.

The conjecture of Elia and Niccoli (2004a) agrees with the QED model of SDVSPL. As noted in paragraphs II-V: At concentrations of about and about two orders of magnitude lower, ions and polar solvent molecules form IPD_plasma. Typically, ~10^-6 M <  <~10^-4 M. For aqueous Na⁺, =2×10^-4 M (Yinnon and Yinnon, 2012). Vigorous shaking of solutions containing IPD_plasma results in formation of EDA^IPDplasma. For C < ,  EDA^IPDplasma can stabilize CD_rot. Typically, 10^-6 M < < 10^-10 M. So indeed according to QED, in SDVSPL-of-polar liquids, the presence of impurities released by the container might induce stabilization of CD_rot. Since dilution, shaking and aging processes alter the alignment of the electric dipoles of CD_rot, these processes affect the stabilization and prevalence of CD_elec. For the UV-vis fluorescence of SDVSPL-of-Distilled-Water, the aforementioned implies that its intensity should vary with each dilution step and with the storage time, just as observed by Lobyshev et al. (2005).

B. Recent developments enable pointing to another source of CD_rot and CD_elec in SDVSPL. In water and other polar liquids, adjacent to the wall of vessel made of glass or other hydrophilic materials, an exclusion zone (EZ) has been shown to form (Zheng et al., 2006; Chai and Pollack, 2010). The analyses by Del Giudice et al. (2013) and Yinnon et al. (2016) have indicated that the EZ contains CD_elec and CD_rot. Just gently stirring of the water adjacent to a hydrophilic surface has been shown to release clumps (aggregates) of ordered H₂O from the EZ (Elia et al., 2013a&b, 2014a, 2015, 2017, 2018; Yinnon et al., 2016). Analyses of the characteristics of these aggregates and their impact on the physicochemical and thermodynamic properties of the liquid have shown that these aggregates have the typical features of supra-CD_rot containing supra- (Yinnon et al., 2016).

The current available experimental data are insufficient for delineating the relative contribution of the two mechanisms to the prevalence of CD_rot and CD_elec in SDVSPL. The hysteretic far-out-of-equilibrium dissipative properties of SDVSPL imply that SDVSPL’s phenomena are repeatable but not quantitatively reproducible. Hence, even the major differences between the UV-vis fluorescence intensity of the first 13 decimally diluted SDVSPL-of-Distilled-Water and aqueous SDVSPL of NaCl, observed by Lobyshev et al. (2005), cannot be simply attributed to the dominance of one of the above described mechanisms. For example, just a difference in the storage time of polar liquids affects the sizes of their EZ adjacent to the wall of the vessel. The accumulation of polar solvent molecules in an EZ is a rather slow process (Zheng et al., 2006; Chai and Pollack, 2010). Typically, after a few seconds, the EZ becomes observable. It grows to a significant size (hundreds of microns) during the first few minutes after the liquid gets into contact with the hydrophilic surface. However, about a day is required for its width to expand to its maximum size. Accordingly, the age of the distilled polar liquid employed for preparing SDVSPL affect their properties. Hence, the prevalence of CD_rot and CD_elec differs even in onetime decimal diluted SDVSPL samples.

Clearance of the abovementioned fuzziness concerning the relative contribution of the two mechanisms seems possible by repeating the UV spectral analyses of Lobyshev et al. (2005) for SDVSPL of NaCl and SDVSPL-of-Distilled-Water prepared and kept in plastic vessels, which do not release impurities and which are closed by plastic lids. Thus, such experiments are called for.

Analyses of UV Radiation Transmission

As shown in the previous paragraphs and previous publications (Lo, 1996; Ryzhkina et al., 2012c; Lobyshev et al. 2005), many investigations of the physicochemical properties of SDVSPL have focussed on aqueous SDVSPL of NaCl. Analyses of the data obtained in these investigations confirmed the various aspects of the QED model of SDVSPL (Yinnon and Liu, 2015b). In particular, the analyses of the UV radiation’s fluorescence by aqueous SDVSPL of NaCl, presented above, indicate that the fluorescence intensity is a function of the prevalence of  . For aqueous SDVSPL of NaCl, the drop in the fluorescence intensity on diluting from 2 M to 2×10^-3 M, we attributed to the decrease in the prevalence of . This decrease is ascribable to the diminishment in the prevalence of the domains composed of Na⁺ and Cl^– ions and H₂O, i.e., the CD_plasma. These domains stabilize . Moreover, the non-monotonic dependence of the fluorescence intensity on the number of dilution steps for concentrations below ≈2×10^-4 M, we attributed to the presence of EDA^IPDplasma which stabilize . For concentrations below ≈10^-7 M, these EDA^IPDplasma stabilize CD_rot, which in turn stabilize . As noted above, the polarization of the liquid caused by CD_rot changes with the number of dilution steps. The polarization affects the stabilization of . Therefore, also the prevalence of changes with the number of dilution steps. According to the aforementioned, the UV radiation’s transmission should increase on diluting SDVSPL of NaCl until C≈10^-4 M. Moreover, it should change non-monotonically with the number of dilution steps for C<10^-4 M. This indeed was observed by Lo (1996). Since the  of aqueous solutions of HNO₃ and NaOH are the same as those of NaCl (Yinnon and Yinnon, 2012), the transmission of UV radiation by aqueous SDVSPL of these liquids should be similar to those of that of aqueous SDVSPL of NaCl. Indeed Lo (1996) observed such a similarity.

As noted above, the UV radiation transmission by aqueous SDVSPL of CuSO₄ or aqueous SDVSPL of hypericum, prepared under the same experimental conditions, is lower than that of the control. In contrast, for aqueous SDVSPL of sublimed S₈, the UV radiation transmission is higher than that of the control. The controls were vigorously shaken, but not diluted water. Since the UV spectral features of SDVSPL have been attributed to the presence of , the UV transmission data indicate that the prevalence of is less in SDVSPL of S₈ than in SDVSPL of CuSO₄ or hypericum. This result implies that the solute affects the . It is plausible that the solute directly impact on the stabilization of .
However, it is also possible that the solute affects the stabilization of CD_rot, which in turn affects the prevalence of .

 

Discussion and Conclusions

The above analyses show that the QED model of SDVSPL consistently explains the UV spectral data. As such, the analyses complement explanations for many types of other physiochemical and structural data which consistently were explained with the model (Yinnon and Yinnon, 2011; Yinnon and Elia, 2013; Yinnon and Liu, 2015b,c; Yinnon, 2017).

The analyses of the absorbance or fluorescence UV spectra do not enable to unambiguously differentiate between the spectra of highly dilute (C<C_thr) SDVSPL prepared with different substrates (i.e., solutes present in the mother solution). The spectra consist of broad featureless bands. The spectra resemble those of various types of structured polar liquids. These structured liquids, just as SDVSPL with C<C_thr, contain nano to micron sized associates mainly composed of the polar liquid molecules. Therefore, studying the absorbance or fluorescence UV spectra of SDVSPL does not facilitate extracting information on the imprint of the properties of the substrate on the electronic structure and molecular organization of the associates present in SDVSPL diluted below C_thr.

UV transmission intensities, in contrast to UV absorbance or fluorescence spectral peaks, do reveal statistically significant differences between extremely diluted SDVSPL prepared with different substrates. Highly controlled experiments showed that there is a difference between the transmission intensities of SDVSPL of copper sulfate (CuSO₄), aqueous SDVSPL of hypericum and aqueous SDVSPL of sublimed sulfur (S₈), which were up to 30 times centesimally diluted (Klein et al., 2013). However, the available transmission data do not reveal the relation between the characteristics of the substrate and the electronic structure and/or molecular organization of the associates present in extremely diluted SDVSPL.

Discovering relations between characteristics of the substrate and properties of their extremely diluted SDVSPL is required for studying the active principle underlying these liquids’ bioactivity. Konovalov and Ryzhkina (2014) showed that for SDVSPL with C<C_thr, their bioactivity is related to their 10² nm associates, which are mainly composed of solvent molecules. On screening SDVSPL from ambient EM fields by placing these liquids in Permalloy containers, their 10² nm associates disintegrate and the liquids’ bioactivity is destroyed. Montagnier et al. (2009, 2011, 2015, 2017a &b) carried out experiments and analyses that provide some additional insights into aspects of the bioactive principle. Firstly, they demonstrated that aqueous SDVSPL of some types of DNA may emit ultra low frequency (ULF) (500-3000 Hz) EM radiation. Such types include DNA from Borrelia burgdorferi or the LTR of HIV-1. The number of dilutions steps required for the SDVSPL to emit the radiation depends on the type of DNA. Typically, at least six decimal dilutions of a few nano gram (ng) of DNA are required for the emission to be detectable. The SDVSPL only emit ULF radiation when these liquids are stimulated by background extremely low frequency (ELF) radiation. The source of the ELF radiation may be the natural Schumann resonances of the geomagnetic field or artificial ones.^g Secondly, they amplified the emitted ULF, digitally recorded it and sent it to a distant laboratory, where they transformed into an analog form. They sent the electric vector of the analog signal to a solenoid, which generated a magnetic field in a test tube of water. They added enzymatic proteins to the water, so as to allow polymerase chain reaction (PCR) processes to occur. They observed that the PCR processes produced and amplified DNA molecules identical to the original DNA (the substrate of the SDVSPL). In other words, the electromagnetic image of the substrate in the SDVSPL is “read” by Taq polymerase in the presence of primers and nucleotide triphosphates. Thirdly, they exposed a flask of living cultured cells to the aforementioned magnetic field. The cells originated from malignant tumors or from isolated in vitro as continuous “immortalized” cell lines. After several days of exposure, the cells synthesized the SDVSPL’s DNA substrate. The synthesis was detected by common PCR procedures. At the same time, the growth of the exposed cells was inhibited and finally they died. Fourthly, they explained their results with the QED model of aqueous systems. They employed the formulism developed by Kurian et al. (2018). They analyzed the electromagnetic image of DNA templated in these molecules’ surrounding water.^h They investigated the spatiotemporal distribution of interaction couplings, frequencies, amplitudes and phase modulations comprising a pattern of fields, such as of the net polarization of water in the vicinity of the DNA. (This net polarization is analogous to the stabilization of CD_rot). They studied the effects of this polarization on dipole modes that can be recognized by Taq polymerase.

So far, to the best of my knowledge, no experimental techniques have been identified which can reveal the relation between substrates’ characteristics and the physicochemical and structural properties of extremely diluted SDVSPL. This, in spite of the fact that extensive and many different types of measurements have been carried out, e.g., electric conductivity, heat of mixing with acids or bases, pH, dielectric permittivity, DLS, nanoparticle tracking analyses, surface tension, impedance, Landau-Placzek ratio, Raman scattering, acoustic, volumetric, viscometric, refractive index, atomic force microscopy, scanning electron microscopy, transmission electron microscopy, fluorescence microscopy, UV, IR, ultra low frequency or nuclear magnetic resonance spectral measurements.

Part of the challenge of uncovering the relation between substrates’ characteristics and the physicochemical and structural properties of extremely diluted SDVSPL is that it has not been derived within the context of QED. This paper’s analyses and previous ones have shown that the QED model of SDVSPL adequately describes many aspects of these liquids; therefore future research should be directed at deriving this relation.

In conclusion, during the last decades and also in the current paper, ample and unambiguous  evidence has been presented that SDVSPL diluted below C_thr may have properties which statistically significantly differ from those of the same liquids which are identically diluted but not vigorously shaken after each dilution step. The QED model of SDVSPL explains this phenomenon. Yet the vast existing experimental data and the theory leave us in the dark as to the relations between the substrates’ characteristics and the bioactive, physicochemical and structural properties of SDVSPL diluted below C_thr. Because of the importance of SDVSPL for pharmacology and agriculture, major theoretical and experimental efforts for elucidating the relations are called for. This requires shifting the last decades’ extensive research emphasis. Instead of demonstrating that the characteristics of SDVSPL may differ from those of the same liquids which are identically diluted but not vigorously shaken, the focus should be the aforementioned relations.

^g The Schumann resonances have frequencies, for example, at 7.83, 14.3, 20.8, 27.3, and 33.8 Hz (Nickolaenko and   Hayakawa, 2002).

^h DNA templating at least some of its properties in its surrounding water has recently been observed by McDermott et al. (2017). They showed that under physiological conditions DNA imprints its chirality on its vicinal water.

 

Acknowledgements

I express my gratitude to Prof. A. M. Yinnon for his continuous support, encouragement and manuscript review. I also express my appreciation and thankfulness to Jesús Aguilar for his careful literature search.

 

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Table  1: List of abbreviations in alphabetic order, followed by Greek symbols abbreviations

Abbrev. /  Explanation

C – Concentration

C_crit – Critical concentration

– Critical concentration below which CDrot may form

– Transition concentration for CD_plasma formation

– Transition concentration for IPD_plasma formation

C_thr – Threshold concentration below which no domains are present in SDVSPL samples screened by Permalloy

CD – Coherence domain

– Coherence domain composed of coherent electronically excited water molecules

CD_plasma – Coherence domain composed of few solvated solutes performing coherent plasma oscillation and numerous polar solvent molecules

CD_rot – Coherence domains of ferroelectric ordered polar solvent molecules

DLS – Dynamic light scattering

EDA^CDrot – Excited or broken CDrot piece, which has an electric dipole moment and therefore is denoted electric dipole aggregate (EDA)

EDA^{IPDplasma –} Excited or broken IPD_plasma piece, which has an electric dipole moment and therefore is denoted electric dipole aggregate (EDA)

EM – Electro-magnetic

ELF – Extremely low frequency

eV – Electron Volt

H2O – Water molecule

Hz – Herz

IPD_plasma – In phase domains composed of few solvated solutes and numerous solvent molecules performing in phase plasma oscillation.

k_B – Boltzmann constant

M – Molarity in mole per liter

m – Meter

mol / l – Mole per Liter

NaCl – Sodium Chloride

nm – Nano-meter

QED – Quantum electro-dynamics

QFE – Quasi free electrons

SDVSPL – Serially diluted vigorously shaken polar liquid

Supra-CD – Agglomerate of coherence domains

ULF – Ultra low frequency

UV – Ultra-violet

Vis – Visible

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Discussion with Reviewers

Reviewer: How is the general frame presented by the author related to the EZ phenomenology of water in the presence of a Nafion film?

Author: The general frame employed by Yinnon and Yinnon (2011) for developing their model of SDVSPL is that of QED. The QED models of aqueous systems and of other polar liquids unambiguously describe electrodynamic forces. These forces span 10^-7 – 10^-4 m. These forces result from the interactions between the EM field and the matter quantum wave field. In contrast, the customary models of polar liquids explicitly describe electro-static forces, but assume that electro-dynamic ones can be treated perturbatively or often even may be ignored. Electrostatic interactions in liquids typically span nm. These interactions result from Coulombic forces between solvent and solute particles.

The need for a QED formulism for developing a model for SDVSPL was recognized by Yinnon and Yinnon (2011). In these liquids up to hundreds of microns sized molecular orderings have been observed (Lo, 1996; Konovalov et al., 2008; Lo et al., 2009; Ryzhkina et al., 2009a&b). The interactions described by the customary models of polar liquids cannot lead to such large orderings (Preparata, 1995). Indeed, the group of Konovalov has shown that interactions between the liquid’s molecules and ambient EM fields are required for formation of the nano- and micron- sized molecular orderings in SDVSPL diluted below the transition concentration C_trh (Ryzhkina et al., 2011a, 2012a). Typically, C_thr is of the order of 10^-6 – 10^-10 M.

The main breakthroughs in the attempts to develop a QED model for polar liquids in general and for water in particular were obtained by Del Giudice, Preparata and Vitiello (1988) and Arani, Bono, Del Giudice and Preparata (1995). These scientists showed that two types of coherent domains may be stabilized in polar liquids. In the main text of this paper, I denoted these domains as CD_rot and CD_elec.

The energy H₂O gain by their inclusion in CD_rot is of the order of the energies of the thermal fluctuations of water at ambient conditions. Therefore, CD_rot do not stabilize in such water. The energy H₂O gain by inclusion in CD_elec is about an order of magnitude larger than the energy of the aforementioned fluctuations. Accordingly, CD_elec are meta-stable in bulk water at ambient conditions.

One of the challenges Yinnon and Yinnon (2011) faced in their pursuit of a QED model of SDVSPL, which is capable of explaining its physicochemical and structural properties, was the following: They had to identify the mechanisms by which CD_rot and CD_elec are stabilized during these liquids preparation procedure. For aqueous solutions of strong or weak electrolytes, they showed that serially diluting up to a transition concentration () leads to formation of a QED domain, denoted as IPD_plasma in the main text. They showed that shaking causes IPD_plasma to transform into aggregates with an electric dipole moment (EDA). On diluting solutions containing EDA below a critical concentration , the EDA stabilize CD_rot and CD_elec. For solutions of non-electrolytic solutes with a sufficiently strong electric dipole, dilution below  also stabilizes CD_rot (Del Giudice et al. 1988; Del Giudice and Vitiello, 2006). These CD_rot can stabilize CD_elec.  These domains underlie these liquids’ physicochemical properties (see main text).

The EZ phenomenology of water in the presence of a Nafion film is the formation of a hundreds of micron wide interfacial water zone. The zone excludes particles such as: medium sized molecules (dyes, acid-base indicators), large molecules (proteins), bacteria, positively or negatively charged colloidal microspheres with diameters of 0.5 – 2.0 µm. Accordingly, it has been denoted Exclusion Zone (EZ). Such a zone forms adjacent to all hydrophilic membranes, as first demonstrated by the group of Pollack (Zheng et al., 2006).

The EZ phenomenology is not explainable with the customary models of aqueous systems. Molecular dynamics simulations solely including electrostatic interactions have been carried out in tandem with experiments. The simulations show H₂O ordering due to their polarization by polar surface groups occurs only up to few nm from hydrophilic surfaces (Buch et al., 2007; Noguchi et al., 2008). EM phenomena pertaining to EZ water entail that modeling effects of interfaces on H₂O ordering warrants inclusion of electrodynamic interactions. Examples of EM phenomena of EZ water include: widening of the zone on irradiation and its narrowing on onset of darkness (Chai et al. 2009). These phenomena are not attributable to temperature changes. Del Giudice et al. (2013) and Yinnon et al. (2016), by employing the QED model of aqueous systems succeeded to explain many physical and structural properties of EZ water. They showed that interactions between H₂O and a Nafion film (or any other hydrophilic membrane) may stabilize CD_rot and CD_elec, i.e., the EZ consists of these domains.

In summary, EZ water and SDVSPL are systems wherein electrodynamic forces play major roles. Therefore, electrodynamic models are required for their description. In both these systems CD_rot and CD_elec are stabilized. Albeit, the mechanisms by which these domains are stabilized differ.

Reviewer: Please, clarify a little more how and if the coherent domains coexist with un-organized (bulk) water.

Author: The energy a H₂O gains on its inclusion in  is about 0.17 eV at a temperature of 273 K and pressure of 1Atm (Bono et al., 2012). Chemical potentials determine the fraction of H₂O included within . In bulk water at T=298 K and pressure of 1Atm, this fraction is about 20 percent. The fraction decreases with increasing temperatures. H₂O, which are not included in , move randomly in between  or evaporate. Continually some of the random moving H₂O adsorb on , while simultaneously others desorb from these domains. These adsorption and desorption process cause a ~10^-14 s timescale flickering landscape. In other words, are meta-stable. Hence, observation of  requires fast resolution probes.  agglomerate in supra-domains. According to the ab initio derived QED model of water, the meta-stable supra- constitute the purely empirically-only based hydrogen-bond network of water (Arani et al., 1995). H₂O are tetrahedrally ordered in . The density of a equals 0.92 g/cm³. The presence of  and randomly moving H₂O in bulk water means that water consists of two phases. The phase consisting of constitutes the low density phase.

Analyses of vast amounts of recent experimental data indicate that bulk water consists of two phases – a high and a low density phase (Nilsson and Pettersson, 2015). However, hitherto, no widely accepted explanations for the molecular orderings in the phases exist. Analyses of the recent data within the context of the QED approach are called for.

The energy a H₂O gains on its inclusion in CD_rot is ~0.025 eV (Del Giudice et al., 2013). For bulk water at ambient conditions k_BT is of this order. Therefore, thermal aggression prevents auto-organization of CD_rot in bulk water. However as noted in the main text, during preparation of an aqueous SDVSPL, CD_rot may stabilize. On continuing serial diluting combined with vigorous shaking of aqueous SDVSPL containing CD_rot, after the Avogadro limit is crossed, the liquid can be considered as bulk water containing CD_rot. Continually, H₂O adsorb and desorb from these CD_rot. Moreover, these CD_rot agglomerate into supra-domains. The CD_rot may organize into supra- CD_rot with their electric dipoles aligned parallel, anti-parallel or oriented in varying directions. Stabilization of CD_rot, the adsorption and desorption of H₂O of these domains, and their agglomeration into supra- CD_rot are very slow processes. Electric conductivity measurements have shown that these processes last at least months or several years (Elia et al., 2008b; Yinnon and Elia, 2013). Supra-CD_rot may stabilize supra-. The latter are encapsulated in the former.

Reviewer: Does the shaking procedure affect the size of the coherent domains?

Author: On shaking 1 liter of SDVSPL for one minute, the energy available for excitation or break-up of aggregates has been estimated to be of the order of 10¹⁸ – 10¹⁹ eV (Yinnon and Liu, 2015b). Gravimetric data indicate that about 1 to 10 percent of the molecules in SDVSPL, which were 45 times decimally diluted, are organized in aggregates (Elia and Napoli, 2010). This implies that the number of associated molecules in one liter of such liquids is of the order of about 10²² – 10²³. A 10^-5 – 10^-4 m sized CD_rot contains about 10¹⁵ – 10¹⁸ H₂O. Accordingly, one liter of aqueous SDVSPL might contain about 10⁴ – 10⁸ CD_rot. Thus 10¹⁸ – 10¹⁹ eV implies 10¹⁰ – 10¹⁵ eV per aggregate. As noted in the previous paragraphs, the energy for desorption of a H₂O from a CD_rot is ~0.025 eV, while the energy of desorption of a H₂O from is ~0.17 eV. The aforementioned numerical analysis indicates that vigorous shaking may tear up CD_rot, supra- CD_rot and . Thus shaking initially reduces the sizes of these domains. However, the H₂O in CD_rot are ferroelectrically ordered. Therefore, broken CD_rot pieces have electric dipole moments, i.e., are electric dipole aggregates (EDA). These enable stabilization of new CD_rot and their agglomeration into supra-CD_rot. These domains may stabilize new .

Reviewer: Explain the relation between the shaking and coherent domain formation.

Author: Several mechanisms, which are triggered by shaking, may be involved in the stabilization of coherent domains in SDVSPL with concentrations below C_trh= . As noted above in the answer to the first question of the reviewer: For aqueous solutions of strong or weak electrolytes, serial diluting up to a transition concentration () leads to formation of IPD_plasma. Shaking causes the IPD_plasma domains to transform into aggregates with an electric dipole moment (EDA^IPDplasma). On diluting the shaken solutions below a critical concentration , the EDA^IPDplasma stabilize CD_rot.  The physics underlying entities with a sufficiently strong electric dipole to stabilize CD_rot has been described by Del Giudice et al., (1988) and Del Giudice and Vitiello (2006). For non-electrolytes, it is not yet known if these can organize into IPD_plasma.  However, for solutions of non-electrolytic solutes with a sufficiently strong electric dipole, dilution below  also stabilizes CD_rot. No shaking is required for stabilization of CD_rot in solutions of electrolytes or non-electrolytes with a sufficiently strong electric dipole when these are diluted below . However, when SDVSPL containing CD_rot are diluted below  without shaking, the concentration of CD_rot diminishes. After many dilution steps, no CD_rot will be present. Rather, for CD_rot to persist in SDVSPL with concentrations far below  or beyond the Avogadro limit, shaking is required. As noted above, shaking tears CD_rot. Broken CD_rot pieces have electric dipole moments, i.e., are electric dipole aggregates (EDA). These enable stabilization of new CD_rot and their agglomeration into supra-CD_rot.