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Dr. Paul Newman Dds

380 N Reservation Rd
Porterville CA 93257
559 842-2316
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License #: 28209
NPI: 1568445385
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Manganese(I) templates for the construction of benzannulated triphosphamacrocycles. - Dalton transactions (Cambridge, England : 2003)
Nine-membered 1,4,7-triphosphamacrocycles with unsaturated benzo-backbones have been prepared using the [(CO)3Mn](+) unit as a template. Two synthetic methods have been employed for the macrocyclisation both of which involve the attack of a coordinated phosphide at an activated, electrophilic ortho-fluorophenyl substituent on a neighbouring pnictide donor. Addition of base to the precursor complex fac-[(CO)3Mn(dfppb)(PhPH2)](+), 1, where dfppb = 1,2-bis[di(2-fluorophenyl)phosphino]benzene, results in the direct formation of the macrocyclic compound fac-[Mn(CO)3(tribenzo-9aneP3-Ph,Ph(F)2)](+), 3. A second precursor, namely fac-[(CO)3Mn(1,2-bpb){P(Ph(F))3}](+), 5, where 1,2-bpb = 1,2-bis(phosphino)benzene, undergoes spontaneous partial macrocyclisation when dissolved in THF to give the intermediate complex fac-[(CO)3Mn{H2PC6H4P(H)C6H4P(Ph(F))2}](+), 6, which contains a linear tridentate phosphine with the unusual combination of a primary, secondary and tertiary phosphine donor. Addition of base to 6 gives the desired macrocyclic complex fac-[Mn(CO)3(tribenzo-9aneP3-H2,Ph(F))](+), 7, which is converted in situ to the more stable dimethylated fac-[Mn(CO)3(tribenzo-9aneP3-Me2,Ph(F))](+), 8. The new complexes have been fully characterised by spectroscopic and analytical methods including single crystal X-ray structure determinations for 1, 3, 5, 6 and 8.
Aspects of the coordination chemistry of rac-trans-1,2-diphosphinocyclohexane and the preparation of reinforced 9aneP₃ and 9anePN₂ macrocycles. - Dalton transactions (Cambridge, England : 2003)
Racemic trans-1,2-diphosphinocyclohexane (t-chxnP2) has been synthesised and its coordination chemistry to Cu(I), Ag(I), Mn(I) and Fe(II) investigated. Compounds of empirical formula [Cu(t-chxnP2)2]BF4 and [Ag(t-chxnP2)2]BF4 have been prepared as isomeric mixtures and the solid-state structure of both complexes determined by single-crystal techniques. The Cu(I) complex is a monomeric species which crystallises with one ligand bearing the R,R configuration and the other being the S,S isomer whereas the Ag(I) complex crystallises as a polymer containing both chelating and bridging t-chxnP2 ligands with 3- and 4-coordinate Ag(I) centres and argentophilic bonds. The bidentate diprimary phosphine has been coordinated to Mn(I) and Fe(II) templates and used as a P2 unit for the formation of chiral (albeit racemic) 1,4,7-triphosphamacrocycles (9aneP3). In addition 1R,2R- and 1R,2S-diaminocyclohexane (chxn) have been coordinated to Mn(I) and Fe(II) templates and similarly employed for the formation of new 1,4-diamino-7-phosphamacrocycle (9anePN2) complexes.
Recent trends in the metabolism and cell biology of vitamin K with special reference to vitamin K cycling and MK-4 biosynthesis. - Journal of lipid research
In contrast to other fat-soluble vitamins, dietary vitamin K is rapidly lost to the body resulting in comparatively low tissue stores. Deficiency is kept at bay by the ubiquity of vitamin K in the diet, synthesis by gut microflora in some species, and relatively low vitamin K cofactor requirements for γ-glutamyl carboxylation. However, as shown by fatal neonatal bleeding in mice that lack vitamin K epoxide reductase (VKOR), the low requirements are dependent on the ability of animals to regenerate vitamin K from its epoxide metabolite via the vitamin K cycle. The identification of the genes encoding VKOR and its paralog VKOR-like 1 (VKORL1) has accelerated understanding of the enzymology of this salvage pathway. In parallel, a novel human enzyme that participates in the cellular conversion of phylloquinone to menaquinone (MK)-4 was identified as UbiA prenyltransferase-containing domain 1 (UBIAD1). Recent studies suggest that side-chain cleavage of oral phylloquinone occurs in the intestine, and that menadione is a circulating precursor of tissue MK-4. The mechanisms and functions of vitamin K recycling and MK-4 synthesis have dominated advances made in vitamin K biochemistry over the last five years and, after a brief overview of general metabolism, are the main focuses of this review.
It's all about Me: methyl-induced control of coordination stereochemistry by a flexible tridentate N,C,N' ligand. - Dalton transactions (Cambridge, England : 2003)
A chiral, tridentate, pyridyl-functionalised NHC pro-ligand, S-L(Me)-H[PF₆], has been prepared diastereoselectively via a five step synthesis starting from 1R,3S-diamino-1,2,2-trimethylcyclopentane. The S prefix refers to the stereochemistry of a methyl substituted stereogenic carbon in one of the pyridyl arms which is generated by a stereoselective BH4(-) reduction of an imine precursor. The ligand has been coordinated to Rh(I) and Ir(I) to give trigonal bipyramidal complexes of the type [M(κ(3)-N,C,N'-S-L(Me))(1,5-COD)]PF6 (M = Rh, Ir) as single diastereomers. A combination of spectroscopic and X-ray techniques confirm the stereoselective formation of the thermodynamically preferred endo,endo isomer. Similar reactions with R,S-L(Me)-H[PF₆] gave a mixture of endo,endo-[M(κ(3)-N,C,N'-S-L(Me))(1,5-COD)](+) and exo,exo-[M(κ(3)-N,C,N'-R-L(Me))(1,5-COD)](+). The absolute configuration at the metal is, therefore, solely dictated by the stereochemistry of the single methylpyridyl carbon. The observation of stereoselection extends to the square planar Ni(II) complex [Ni(δ-κ(3)-N,C,N'-S-L(Me))Cl](+) which is isolated as one (δ) of the two possible conformational isomers. DFT studies have been employed to explain the observed stereoselectivity with the configurations observed in the solid state being confirmed as those of lowest energy.
Evolution of physician-hospital alignment models: a case study of comanagement. - Clinical orthopaedics and related research
Recently, quality, financial, and regulatory demands have driven physicians to seek alignment opportunities with hospitals. The motivation for alignment on the part of physicians and hospitals is now accelerating because the new paradigm under healthcare reform requires an increased focus on improving quality, cost, and efficiency.We (1) identify the key drivers for physician-hospital alignment models; (2) summarize comanagement as a physician-hospital alignment model; and (3) explore a detailed case study of comanagement as an option to better align physicians with hospital goals on quality, safety, and outcomes.A Medline abstract review was performed that identified 45 references that discuss options for physician-hospital alignment. None of the articles identified provide a detailed example of successful alignment structures. A detailed case study of a successful comanagement alignment program is reviewed.The key drivers for alignment are inpatient growth rates, declining reimbursements, and the opportunity to improve quality, decrease costs, and increase efficiency. Two general strategies of alignment involve noneconomic and/or economic integration. In our example, comanagement with economic integration was chosen as the preferred structure for physician-hospital alignment.The choice of structure will vary depending on the existing relationships and governance of the hospital and the physicians in the targeted area of focus. The measure of success in building physician-hospital alignment is measured in improvements in care for the patient, reduced cost of care delivery, and improved relations between physicians and hospital leadership.
Variable coordination of a chiral diphosphine containing an amidinium/NHC group within its backbone: μ-P,P', κ2-P,P' and κ3-P,C,P' coordination modes. - Dalton transactions (Cambridge, England : 2003)
A diphosphine ligand (1·HPF(6)), which is a potential precursor to a PC(NHC)P pincer, with a backbone containing two phenylene groups and a central bicyclic 4-aza-2-azoniabicyclo[3.2.1]oct-2-ene unit has been synthesised and coordinated to Pd(II) and Pt(II) to give trans-[M(κ(2)-P,P'-)Cl(2)]PF(6) where M = Pd (2) or Pt (3a). Single-crystal structure determinations of 2 and 3a show the complexes to be isostructural with the diphosphine coordinated in a trans-spanning fashion and the amidinium unit being protonated and non-coordinated. 2 and 3a react with CH(3)I to give the dimers trans-[Pd(2)(μ-1·H)(2)I(4)](PF(6))(2), 6, and trans-[Pt(2)(μ-1·H)(2)I(4)](PF(6))(2), 7, as the major products. This bridging mode of coordination of [1·H](+) is also seen in trans-[Rh(2)(μ-1·H)(1,5-COD)(2)Cl(2)]PF(6), 4, and [Pt(2)(μ-κ(2)-1·H)(dvdms)]PF(6), 5. Upon treatment with KO(t)Bu complexes and undergo deprotonation at the amidinium carbon to give trans-[M(κ(3)-P,C,P'-1)Cl]PF(6) where M = Pd (8), and Pt (9). The related trans-[Rh(κ(3)-P,C,P'-1)(CO)]PF(6) (10) is prepared directly from 1·HPF(6) and Rh(acac)(CO)(2): this and the palladium and platinum complexes 8 and 9 are isolated as isomeric mixtures as a consequence of a conformational isomerism. In situ deprotonation of 1·HPF(6) followed by addition of Ag(CF(3)SO(3)) gave S(Ag)-[Ag(κ(3)-P,C,P'-1)(CF(3)SO(3))], 11. Some preliminary studies of the reactivity of 2 and 8 in Suzuki-type reactions are reported and the Pt(0) system has been shown to be an active hydrosilylation catalyst.
Monovalent chiral-at-copper complexes: halide-controlled diastereoselectivity. - Chemical communications (Cambridge, England)
An unusual example of diastereoselectivity has been observed in Cu(κ(3)-P,C,P'-1)X complexes where 1 is an asymmetric tridentate ligand containing a bicyclic NHC framework and X is a halide. When X is Cl(-), the S(Cu) isomer is formed selectively whereas when X = I(-) the R(Cu) diastereomer is preferred.
Association of vitamin K status with adiponectin and body composition in healthy subjects: uncarboxylated osteocalcin is not associated with fat mass and body weight. - The British journal of nutrition
Osteocalcin (OC) is a vitamin K-dependent protein found in bone and in circulation. High serum γ-carboxylated OC reflects a high, and high uncarboxylated OC (ucOC) reflects a low vitamin K status. A revolutionary hypothesis is that ucOC acts as a hormone improving glucose handling and reducing fat mass. The objective was to test the logical extrapolation of the ucOC hormone hypothesis to humans that elevated ucOC is associated with higher body weight, BMI and fat mass. In a cross-sectional analysis, the associations of vitamin K status with circulating adiponectin and body composition were investigated in 244 postmenopausal women (study I). The effects of vitamin K treatment on adiponectin, body weight and BMI were investigated in archived samples from forty-two young men and women who received varying doses of menaquinone-7 during 12 weeks (study II) and from a cohort of 164 postmenopausal women who participated in a 3-year placebo-controlled trial on 45 mg menaquinone-4 (MK-4) (study III). No association was found between vitamin K status and circulating adiponectin before or after vitamin K supplementation. A higher carboxylation of OC was significantly correlated with lower body weight, BMI and fat mass of the trunk. Women taking MK-4 maintained their baseline body weight and BMI, whereas women taking placebo showed significant increases in both indices. These findings demonstrate that a high vitamin K status of bone has no effect on circulating adiponectin in healthy people and long-term vitamin K supplementation does not increase weight in healthy postmenopausal women.
Iron(II) template synthesis of benzannulated triphospha- and triarsamacrocycles. - Dalton transactions (Cambridge, England : 2003)
Nine-membered 1,4,7-triphospha- and triarsamacrocycles with unsaturated benzo-backbones have been prepared using the [Cp(R)Fe](+) unit as a template. The cyclisation involves the attack of a coordinated phosphide (or arsenide) nucleophile at an activated, electrophilic ortho-fluorophenyl substituent on a neighbouring pnictide donor. The macrocycle assembly is of the 2 + 1 type where two new chelate rings are formed from appropriately derivatised bidentate and monodentate phosphines/arsines. Both [(η(5)-C(5)H(5))Fe](+) and [(η(5)-C(5)Me(5))Fe](+) may be employed for the cyclisation with higher yields generally being observed with the unsubstituted Cp. All new compounds have been characterised by spectroscopic and analytical methods including the single-crystal X-ray structure determination of [(η(5)-C(5)H(5))Fe(tribenzo-9aneP(3)-Ph,Ph(F)(2))](+), 3a, and [(η(5)-C(5)H(5))Fe(tribenzo-9aneAs(3)-Ph,Ph(F)(2))](+), 5, as the tetraphenylborate salts. The crystal structures are isomorphous and show the unique conformation of these new macrocycles with a 'cup shaped' cavity formed by the rigid benzo-backbones. The 9aneAs(3) derivative is the first example of a nine-membered triarsamacrocycle.
Rhodium and iridium complexes of an asymmetric bicyclic NHC bearing secondary pyridyl donors. - Dalton transactions (Cambridge, England : 2003)
A tridentate N^C^N ligand, 1, containing a bicyclic central NHC ring and two flanking pyridyl groups has been coordinated to Rh(I) and Ir(I) to give complexes of the type [M(κ(3)-1)(1,5-COD)]PF(6) (2 M = Rh; 3 M = Ir). In contrast to our earlier study with this ligand, the complexes have been shown to approximate to a trigonal bipyramidal geometry in the solid state and exist as an isomeric mixture in solution as determined by (1)H and (13)C NMR spectroscopy. Electrochemical studies revealed that both complexes undergo a 1-electron oxidation with the potential of the Rh complex 0.1 V less than that of the Ir complex in CH(2)Cl(2). Preliminary DFT studies confirm the lowest energy conformations as those seen in the solid state and show the location and energy of the HOMOs to be identical in 2 and 3. Partial charge analysis shows a greater positive charge on the Ir in 3 compared to the Rh in 2. Some preliminary studies of hydrogenation reactivity have shown the complexes to be efficient for both transfer and direct hydrogenation of prochiral ketones and alkenes at moderate temperatures but without any discernible enantioselectivity.This journal is © The Royal Society of Chemistry 2011

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