Hydrogel microrheology near the liquid-solid transition

Travis Larsen; Kelly Schultz; Eric M. Furst

Korea-Australia Rheology Journal, Vol.20, No.3, 165-173, September, 2008

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Hydrogel microrheology near the liquid-solid transition

Travis Larsen, Kelly Schultz, and Eric M. Furst^†

Department of Chemical Engineering and Center for Molecular and Engineering Thermodynamics, University of Delaware, Newark, DE 19716, USA

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Multiple particle tracking microrheology is used to characterize the viscoelastic properties of biomaterial and synthetic polymer gels near the liquid-solid transition. Probe particles are dispersed in the gel precursors, and their dynamics are measured as a function of the extent of reaction during gel formation. We interpret the dynamics using the generalized Stokes-Einstein relationship (GSER), using a form of the GSER that emphasizes the relationship between the probe particle mean-squared displacement and the material creep compliance. We show that long-standing concepts in gel bulk rheology are applicable to microrheological data, including time-cure superposition to identify the gel point and critical scaling exponents, and the power-law behavior of incipient network's viscoelastic response. These experiments provide valuable insight into the rheology, structure, and kinetics of gelling materials, and are especially powerful for studying the weak incipient networks of dilute gelators, as well as scarce materials, due to the small sample size requirements and rapid data acquisition.

Keywords:hydrogel;peptide;microrheology;particle tracking;superposition;critical gel

[References]

Adolf D, Martin JE, Macromolecules, 23, 3700 (1990)
Bobroff N, Rev. Sci. Instrum., 57, 1152 (1986)
Chin K, Vacanti JP, Biotech. Prog., 24, 358 (2008)
Crocker JC, Grier DG, J. Colloid Interface Sci., 179(1), 298 (1996)
Davis ME, Motion JPM, Narmoneva DA, Takahashi T, Hakuno D, Kamm RD, Zhang SG, Lee RT, Circulation, 111, 442 (2005)
Davis MW, Vacanti JP, Biomaterials, 17, 365 (1996)
Derrida B, Stauffer D, Herrmann HJ, Vannimenus J, J.Phys. Lett. (France), 44, L701 (1983)
Ellis-Behnke RG, Liang YX, You SW, Tay DKC, Zhang SG, So KF, Schneider GE, Proc. Natl. Acad. Sci. USA, 103, 5054 (2006)
Ferry J, 1980, Viscoelastic properties of polymers, Wiley, New York
Gardel ML, Valentine MT, Crocker JC, Bausch AR, Weitz DA, Phys. Rev. Lett., 91, 158302 (2003)
Grinstaff MW, Biomaterials, 28, 5205 (2007)
Haines-Butterick L, Rajagopal K, Branco M, Salick D, Rughani R, Pilarz M, Lamm MS, Pochan DJ, Schneider JP, Proc. Natl. Acad. Sci., 104, 7791 (2007)
Hoffman AS, Adv. Drug Delivery Rev., 43, 3 (2002)
Joanny JF, J. Phys. (France), 43, 467 (1982)
Langer R, Peppas NA, AIChE J., 49(12), 2990 (2003)
Larsen TH, Furst EM, Phys. Rev. Lett., 100, 146001 (2008)
Lee KY, Mooney DJ, Chem. Rev., 101(7), 1869 (2001)
Lutolf MP, Hubbell JA, Nat. Biotechnol., 23, 47 (2005)
Martin JE, Adolf D, Wilcoxon JP, Phys. Rev. Lett., 61, 2620 (1988)
Martin JE, Adolf D, Wilcoxon JP, Phys. Rev. A, 39, 1325 (1989)
Mason TG, Rheol. Acta, 39(4), 371 (2000)
Mikos AG, Herring SW, Ochareon P, Elisseeff J, Lu HH, Kandel R, Schoen FJ, Toner M, Mooney D, Atala A, Van Dyke ME, Kaplan D, Vunjak-Novakovic G, Tissue Engineering, 12, 3307 (2006)
Nie T, Baldwin A, Yamaguchi N, Kiick KL, J. Controlled Release, 122, 287 (2007)
Ozbas B, Kretsinger J, Rajagopal K, Schneider JP, Pochan DJ, Macromolecules, 37(19), 7331 (2004)
Palmer A, Xu JY, Wirtz D, Rheol. Acta, 37(2), 97 (1998)
Peppas NA, Bures P, Leobandung W, Ichikawa H, Eur. J. Pharmacol. Biopharm., 50, 27 (2000)
Pochan DJ, Schneider JP, Kretsinger J, Ozbas B, Rajagopal K, Haines L, J. Am. Chem. Soc., 125(39), 11802 (2003)
Rajagopal K, Schneider JP, Curr. Opin. Struct. Biol., 14, 480 (2004)
Savin T, Doyle PS, Biophys. J., 88, 623 (2005)
Savin T, Doyle PS, Soft Matter, 3, 1194 (2007)
Scanlan JC, Winter HH, Macromolecules, 24, 47 (1991)
Schneider JP, Pochan DJ, Ozbas B, Rajagopal K, Pakstis L, Kretsinger J, J. Am. Chem. Soc., 124(50), 15030 (2002)
Stauffer D, Coniglio A, Adam M, Adv. Polym. Sci., 44, 103 (1982)
Stevens MM, George JH, Science, 310, 1135 (2005)
Tseng Y, An KM, Wirtz D, J. Biol. Chem., 277, 18143 (2002)
Veerman C, Rajagopal K, Palla CS, Pochan DJ, Schneider JP, Furst EM, Macromolecules, 39(19), 6608 (2006)
Winter HH, Chambon F, J. Rheol., 30, 367 (1986)
Winter HH, Chambon F, J. Rheol., 31, 683 (1987)
Winter HH, Mours M, Adv. Polym. Sci., 134, 165 (1997)
Wu DQ, Sun YX, Xu XD, Cheng SX, Zhang XZ, Zhuo RX, Biomacro., 9, 1155 (2008)
Xu CY, Breedveld V, Kopecek J, Biomacromolecules, 6(3), 1739 (2005)
Zimenkov Y, Dublin SN, Ni R, Tu RS, Breedveld V, Apkarian RP, Conticello VP, J. Am. Chem. Soc., 128(21), 6770 (2006)

[1] Adolf D, Martin JE, Macromolecules, 23, 3700 (1990)

[2] Bobroff N, Rev. Sci. Instrum., 57, 1152 (1986)

[3] Chin K, Vacanti JP, Biotech. Prog., 24, 358 (2008)

[4] Crocker JC, Grier DG, J. Colloid Interface Sci., 179(1), 298 (1996)

[5] Davis ME, Motion JPM, Narmoneva DA, Takahashi T, Hakuno D, Kamm RD, Zhang SG, Lee RT, Circulation, 111, 442 (2005)

[6] Davis MW, Vacanti JP, Biomaterials, 17, 365 (1996)

[7] Derrida B, Stauffer D, Herrmann HJ, Vannimenus J, J.Phys. Lett. (France), 44, L701 (1983)

[8] Ellis-Behnke RG, Liang YX, You SW, Tay DKC, Zhang SG, So KF, Schneider GE, Proc. Natl. Acad. Sci. USA, 103, 5054 (2006)

[9] Ferry J, 1980, Viscoelastic properties of polymers, Wiley, New York

[10] Gardel ML, Valentine MT, Crocker JC, Bausch AR, Weitz DA, Phys. Rev. Lett., 91, 158302 (2003)

[11] Grinstaff MW, Biomaterials, 28, 5205 (2007)

[12] Haines-Butterick L, Rajagopal K, Branco M, Salick D, Rughani R, Pilarz M, Lamm MS, Pochan DJ, Schneider JP, Proc. Natl. Acad. Sci., 104, 7791 (2007)

[13] Hoffman AS, Adv. Drug Delivery Rev., 43, 3 (2002)

[14] Joanny JF, J. Phys. (France), 43, 467 (1982)

[15] Langer R, Peppas NA, AIChE J., 49(12), 2990 (2003)

[16] Larsen TH, Furst EM, Phys. Rev. Lett., 100, 146001 (2008)

[17] Lee KY, Mooney DJ, Chem. Rev., 101(7), 1869 (2001)

[18] Lutolf MP, Hubbell JA, Nat. Biotechnol., 23, 47 (2005)

[19] Martin JE, Adolf D, Wilcoxon JP, Phys. Rev. Lett., 61, 2620 (1988)

[20] Martin JE, Adolf D, Wilcoxon JP, Phys. Rev. A, 39, 1325 (1989)

[21] Mason TG, Rheol. Acta, 39(4), 371 (2000)

[22] Mikos AG, Herring SW, Ochareon P, Elisseeff J, Lu HH, Kandel R, Schoen FJ, Toner M, Mooney D, Atala A, Van Dyke ME, Kaplan D, Vunjak-Novakovic G, Tissue Engineering, 12, 3307 (2006)

[23] Nie T, Baldwin A, Yamaguchi N, Kiick KL, J. Controlled Release, 122, 287 (2007)

[24] Ozbas B, Kretsinger J, Rajagopal K, Schneider JP, Pochan DJ, Macromolecules, 37(19), 7331 (2004)

[25] Palmer A, Xu JY, Wirtz D, Rheol. Acta, 37(2), 97 (1998)

[26] Peppas NA, Bures P, Leobandung W, Ichikawa H, Eur. J. Pharmacol. Biopharm., 50, 27 (2000)

[27] Pochan DJ, Schneider JP, Kretsinger J, Ozbas B, Rajagopal K, Haines L, J. Am. Chem. Soc., 125(39), 11802 (2003)

[28] Rajagopal K, Schneider JP, Curr. Opin. Struct. Biol., 14, 480 (2004)

[29] Savin T, Doyle PS, Biophys. J., 88, 623 (2005)

[30] Savin T, Doyle PS, Soft Matter, 3, 1194 (2007)

[31] Scanlan JC, Winter HH, Macromolecules, 24, 47 (1991)

[32] Schneider JP, Pochan DJ, Ozbas B, Rajagopal K, Pakstis L, Kretsinger J, J. Am. Chem. Soc., 124(50), 15030 (2002)

[33] Stauffer D, Coniglio A, Adam M, Adv. Polym. Sci., 44, 103 (1982)

[34] Stevens MM, George JH, Science, 310, 1135 (2005)

[35] Tseng Y, An KM, Wirtz D, J. Biol. Chem., 277, 18143 (2002)

[36] Veerman C, Rajagopal K, Palla CS, Pochan DJ, Schneider JP, Furst EM, Macromolecules, 39(19), 6608 (2006)

[37] Winter HH, Chambon F, J. Rheol., 30, 367 (1986)

[38] Winter HH, Chambon F, J. Rheol., 31, 683 (1987)

[39] Winter HH, Mours M, Adv. Polym. Sci., 134, 165 (1997)

[40] Wu DQ, Sun YX, Xu XD, Cheng SX, Zhang XZ, Zhuo RX, Biomacro., 9, 1155 (2008)

[41] Xu CY, Breedveld V, Kopecek J, Biomacromolecules, 6(3), 1739 (2005)

[42] Zimenkov Y, Dublin SN, Ni R, Tu RS, Breedveld V, Apkarian RP, Conticello VP, J. Am. Chem. Soc., 128(21), 6770 (2006)