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Volumn 128, Issue 19, 2008, Pages

Free-energy analysis of the molecular binding into lipid membrane with the method of energy representation

Author keywords

[No Author keywords available]

Indexed keywords

CHEMICAL BONDS; COMPUTER SIMULATION; FREE ENERGY; HYDROPHOBICITY; MOLECULAR DYNAMICS; SOLVATION;

EID: 44349122912     PISSN: 00219606     EISSN: None     Source Type: Journal    
DOI: 10.1063/1.2919117     Document Type: Article
Times cited : (69)

References (89)
  • 1
    • 85059500208 scopus 로고    scopus 로고
    • 2nd ed., edited by P. L. Yeagle (CRC, Boca Raton, FL).
    • The Structure of Biological Membranes, 2nd ed., edited by, P. L. Yeagle, (CRC, Boca Raton, FL, 2005).
    • (2005) The Structure of Biological Membranes
  • 3
    • 0016258172 scopus 로고
    • 0022-2631 10.1007/BF01870175.
    • Y. Katz and J. M. Diamond, J. Membr. Biol. 0022-2631 10.1007/BF01870175 17, 101 (1974).
    • (1974) J. Membr. Biol. , vol.17 , pp. 101
    • Katz, Y.1    Diamond, J.M.2
  • 4
    • 0017125226 scopus 로고
    • 0022-1295 10.1085/jg68.2.127.
    • A. Finkelstein, J. Gen. Physiol. 0022-1295 10.1085/jgp.68.2.127 68, 127 (1976).
    • (1976) J. Gen. Physiol. , vol.68 , pp. 127
    • Finkelstein, A.1
  • 7
    • 0024285006 scopus 로고
    • 0006-2960 10.1021/bi00414a050.
    • L. R. De Young and K. A. Dill, Biochemistry 0006-2960 10.1021/bi00414a050 27, 5281 (1988).
    • (1988) Biochemistry , vol.27 , pp. 5281
    • De Young, L.R.1    Dill, K.A.2
  • 11
    • 0034318823 scopus 로고    scopus 로고
    • 1089-5647 10.1021/jp001540l.
    • P. Westh and C. Trandum, J. Phys. Chem. B 1089-5647 10.1021/jp001540l 104, 11334 (2000).
    • (2000) J. Phys. Chem. B , vol.104 , pp. 11334
    • Westh, P.1    Trandum, C.2
  • 17
  • 19
    • 0033019968 scopus 로고    scopus 로고
    • 0006-3495
    • B. Roux, Biophys. J. 77, 139 (1999). 0006-3495
    • (1999) Biophys. J. , vol.77 , pp. 139
    • Roux, B.1
  • 20
  • 29
  • 30
    • 0037158526 scopus 로고    scopus 로고
    • 0021-9606 10.1063/1.1495850, ();, J. Chem. Phys. 0021-9606 10.1063/1.1533752 118, 2446 (2003).
    • N. Matubayasi and M. Nakahara, J. Chem. Phys. 0021-9606 10.1063/1.1495850 117, 3605 (2002); N. Matubayasi and M. Nakahara, J. Chem. Phys. 0021-9606 10.1063/1.1533752 118, 2446 (2003).
    • (2002) J. Chem. Phys. , vol.117 , pp. 3605
    • Matubayasi, N.1    Nakahara, M.2    Matubayasi, N.3    Nakahara, M.4
  • 31
  • 35
    • 0036667740 scopus 로고    scopus 로고
    • 0959-440X 10.1016/S0959-440X(02)00353-6.
    • H. L. Scott, Curr. Opin. Struct. Biol. 0959-440X 10.1016/S0959-440X(02) 00353-6 12, 495 (2002).
    • (2002) Curr. Opin. Struct. Biol. , vol.12 , pp. 495
    • Scott, H.L.1
  • 37
    • 0036286655 scopus 로고    scopus 로고
    • 0001-4842 10.1021/ar010167c.
    • L. Saiz and M. L. Klein, Acc. Chem. Res. 0001-4842 10.1021/ar010167c 35, 482 (2002).
    • (2002) Acc. Chem. Res. , vol.35 , pp. 482
    • Saiz, L.1    Klein, M.L.2
  • 44
    • 0032614136 scopus 로고    scopus 로고
    • 0021-9606 10.1063/1.479313.
    • S. E. Feller and R. W. Pastor, J. Chem. Phys. 0021-9606 10.1063/1.479313 111, 1281 (1999).
    • (1999) J. Chem. Phys. , vol.111 , pp. 1281
    • Feller, S.E.1    Pastor, R.W.2
  • 50
    • 44349185874 scopus 로고    scopus 로고
    • The drawback of the approach is that the solvation free energy is evaluated from an approximate functional.
    • The drawback of the approach is that the solvation free energy is evaluated from an approximate functional.
  • 52
    • 44349112088 scopus 로고    scopus 로고
    • The one-to-one association is implied in Eq.. This is because both the membrane and solute are assumed to be dilute in the present formulation. When more than one solute molecule is involved in the membrane solution, it suffices to extend the development straightforwardly by viewing one of the solute molecules as the "solute" species and the others as the "solvent" species constituting the "mixed solvent" system.
    • The one-to-one association is implied in Eq.. This is because both the membrane and solute are assumed to be dilute in the present formulation. When more than one solute molecule is involved in the membrane solution, it suffices to extend the development straightforwardly by viewing one of the solute molecules as the "solute" species and the others as the "solvent" species constituting the "mixed solvent" system.
  • 53
    • 44349103372 scopus 로고    scopus 로고
    • The extension of the formulation is straightforward when the system contains cosolvents.
    • The extension of the formulation is straightforward when the system contains cosolvents.
  • 54
    • 44349167431 scopus 로고    scopus 로고
    • The condition of a fixed (total) chemical potential of the solute is realized, for example, when the counterpart of the equilibrium of the solute insertion is common to the membrane solution and neat solvent.
    • The condition of a fixed (total) chemical potential of the solute is realized, for example, when the counterpart of the equilibrium of the solute insertion is common to the membrane solution and neat solvent.
  • 55
    • 44349181759 scopus 로고    scopus 로고
    • When S (0) (Km + Vm) is much larger than nA, Kx is simply close to Cw /S (0) and is determined essentially by the solubility in the neat solvent. Indeed, when the affinity of the solute to the membrane is strong enough, the mole fraction in the membrane is at the order of 1 and the order of Kx is given by the solubility in neat water for a sparingly soluble solute. In this case, Kx (or Δ Gx) is not very informative for the solute-membrane correlation.
    • When S (0) (Km + Vm) is much larger than nA, Kx is simply close to Cw /S (0) and is determined essentially by the solubility in the neat solvent. Indeed, when the affinity of the solute to the membrane is strong enough, the mole fraction in the membrane is at the order of 1 and the order of Kx is given by the solubility in neat water for a sparingly soluble solute. In this case, Kx (or Δ Gx) is not very informative for the solute-membrane correlation.
  • 56
    • 33751132430 scopus 로고
    • 0021-9606 10.1063/1.1748352.
    • J. G. Kirkwood and F. P. Buff, J. Chem. Phys. 0021-9606 10.1063/1.1748352 19, 774 (1951).
    • (1951) J. Chem. Phys. , vol.19 , pp. 774
    • Kirkwood, J.G.1    Buff, F.P.2
  • 57
  • 58
    • 44349110441 scopus 로고    scopus 로고
    • In Eq., one membrane aggregate is treated as a single particle. The configuration fluctuates within the aggregate, and the coordinates for the intra-aggregate motion are incorporated in the definition of x.
    • In Eq., one membrane aggregate is treated as a single particle. The configuration fluctuates within the aggregate, and the coordinates for the intra-aggregate motion are incorporated in the definition of x.
  • 59
    • 44349193748 scopus 로고    scopus 로고
    • Actually, an arbitrary position in the solute molecule can be taken as the molecular center. The Gsm /A value calculated from Eq. or is independent of the choice of the molecular center of the solute.
    • Actually, an arbitrary position in the solute molecule can be taken as the molecular center. The Gsm /A value calculated from Eq. or is independent of the choice of the molecular center of the solute.
  • 60
    • 33748658848 scopus 로고    scopus 로고
    • 0022-3654 10.1021/jp951618b.
    • N. Matubayasi and R. M. Levy, J. Phys. Chem. 0022-3654 10.1021/jp951618b 100, 2681 (1996).
    • (1996) J. Phys. Chem. , vol.100 , pp. 2681
    • Matubayasi, N.1    Levy, R.M.2
  • 65
    • 44349184643 scopus 로고    scopus 로고
    • manuscript in preparation. The equilibration scheme adopted is summarized as follows. First, 128 DMPC molecules were placed in lattice form with the conformation at the crystal phase. Then 3405 water molecules were added, and the system was equilibrated through an 80 ns molecular dynamics simulation in the N Pn AT ensemble with the membrane area corresponding to the experimental value (Ref.). Finally, the number of water molecules was increased to 3886 and the equilibration was further performed for 6 ns.
    • W. Shinoda and M. L. Klein, manuscript in preparation. The equilibration scheme adopted is summarized as follows. First, 128 DMPC molecules were placed in lattice form with the conformation at the crystal phase. Then 3405 water molecules were added, and the system was equilibrated through an 80 ns molecular dynamics simulation in the N Pn AT ensemble with the membrane area corresponding to the experimental value (Ref.). Finally, the number of water molecules was increased to 3886 and the equilibration was further performed for 6 ns.
    • Shinoda, W.1    Klein, M.L.2
  • 69
    • 44349107364 scopus 로고    scopus 로고
    • note
    • The area compressibility modulus is given by kB T 〈A〉 / 〈 δ A2 〉, where 〈A〉 is the average of the total area of the membrane and 〈 δ A2 〉 is its mean square deviation (Ref.). When the experimental value of 234 dyne/cm is used for the modulus (Ref.) and the membrane area is considered to be ∼60 Å2 per lipid, 〈 δ A2 〉 is ∼80 Å2 with 128 DMPC molecules and is larger than the area expected to be occupied by the solute treated in the present work. According to the membrane simulations involving alcoholic or anesthetic solute (Refs.), the membrane area changes by a few percent when the mole ratio of the solute to the phospholipid is ∼0.1. In our simulation, the mole ratio is 1/128 (a single solute molecule in 128 DMPC molecules). The area expansion or contraction is thus negligible upon introduction of CO, CO2, benzene, or ethylbenzene as the solute; the area can be safely taken to be identical between the solution and reference solvent systems.
  • 70
    • 26144434487 scopus 로고
    • 0031-9007 10.1103/PhysRevLett.45.1196.
    • M. Parrinello and A. Rahman, Phys. Rev. Lett. 0031-9007 10.1103/PhysRevLett.45.1196 45, 1196 (1980).
    • (1980) Phys. Rev. Lett. , vol.45 , pp. 1196
    • Parrinello, M.1    Rahman, A.2
  • 73
    • 0037693091 scopus 로고    scopus 로고
    • 0192-8651 10.1002/jcc.10249.
    • W. Shinoda and M. Mikami, J. Comput. Chem. 0192-8651 10.1002/jcc.10249 24, 920 (2003).
    • (2003) J. Comput. Chem. , vol.24 , pp. 920
    • Shinoda, W.1    Mikami, M.2
  • 74
    • 44349097212 scopus 로고    scopus 로고
    • For all the solutes and the regions of solute position, ρ k,0 e and kl,0 e can be constructed from a single trajectory of the membrane system without the solute since the solute insertion as a test particle does not affect the trajectory. This is useful to reduce the computational demand when a multiple set of solvations is to be treated against a common (mixed) solvent system. A similar remark applies to the calculation in neat water.
    • For all the solutes and the regions of solute position, ρ k,0 e and kl,0 e can be constructed from a single trajectory of the membrane system without the solute since the solute insertion as a test particle does not affect the trajectory. This is useful to reduce the computational demand when a multiple set of solvations is to be treated against a common (mixed) solvent system. A similar remark applies to the calculation in neat water.
  • 75
    • 48749148224 scopus 로고
    • 0021-9991 10.1016/0021-9991(83)90014-1.
    • H. C. Andersen, J. Comput. Phys. 0021-9991 10.1016/0021-9991(83)90014-1 52, 24 (1983).
    • (1983) J. Comput. Phys. , vol.52 , pp. 24
    • Andersen, H.C.1
  • 76
    • 44349178980 scopus 로고    scopus 로고
    • The free energies presented in Ref. are different from those in this work. According to the notation in Eq. (2) of Ref., Jedlovszky and Mezei showed A′ in their paper while we show μ.
    • The free energies presented in Ref. are different from those in this work. According to the notation in Eq. (2) of Ref., Jedlovszky and Mezei showed A′ in their paper while we show μ′.
  • 77
    • 44349087905 scopus 로고    scopus 로고
    • The cavity-insertion Widom method is highly efficient when it works. When the solute size is large, however, an appropriate cavity is not found in the molecular simulation system and the method does not work. For the DMPC-water system, benzene and ethylbenzene are too large and are beyond the applicability of the cavity-insertion Widom method. In the approximate procedure described in Secs., the overlapping configuration produced upon the solute insertion provides nonzero ρ k,0 e and kl,0 e at large energy coordinates and contributes to the solvation free energy as the excluded-volume effect.
    • The cavity-insertion Widom method is highly efficient when it works. When the solute size is large, however, an appropriate cavity is not found in the molecular simulation system and the method does not work. For the DMPC-water system, benzene and ethylbenzene are too large and are beyond the applicability of the cavity-insertion Widom method. In the approximate procedure described in Secs., the overlapping configuration produced upon the solute insertion provides nonzero ρ k,0 e and kl,0 e at large energy coordinates and contributes to the solvation free energy as the excluded-volume effect.
  • 78
    • 44349124858 scopus 로고    scopus 로고
    • note
    • When the solvation free energy is given by Δμ (z) as a continuous function of z and the region of interest is identified as A
  • 79
    • 44349139816 scopus 로고    scopus 로고
    • The contributions to Kx from regions V-VI are 0.09%, 0.7%, 0.04%, and 0.001% in weight for CO, CO2, benzene, and ethylbenzene, respectively.
    • The contributions to Kx from regions V-VI are 0.09%, 0.7%, 0.04%, and 0.001% in weight for CO, CO2, benzene, and ethylbenzene, respectively.
  • 80
    • 44349160411 scopus 로고    scopus 로고
    • The discussion concerning Δμ is based on the approximation expressed as Eqs.. The arguments concerning 〈u〉 are exact within the statistical error, on the other hand, for the potential functions employed.
    • The discussion concerning Δμ is based on the approximation expressed as Eqs.. The arguments concerning 〈u〉 are exact within the statistical error, on the other hand, for the potential functions employed.
  • 81
    • 22944437769 scopus 로고    scopus 로고
    • 0021-9606 10.1063/1.1849165.
    • N. Matubayasi and M. Nakahara, J. Chem. Phys. 0021-9606 10.1063/1.1849165 122, 074509 (2005).
    • (2005) J. Chem. Phys. , vol.122 , pp. 074509
    • Matubayasi, N.1    Nakahara, M.2
  • 82
    • 44349146987 scopus 로고    scopus 로고
    • As shown in Refs., the density dependence is steefor the contribution from the repulsive component of the solute-solvent interaction to the solvation free energy, while it is milder for the contribution from the attractive component. Correspondingly, when the water density decreases in the interfacial region of the membrane, the reduction of the repulsive effect is stronger and the solvation free energy can be negative.
    • As shown in Refs., the density dependence is steep for the contribution from the repulsive component of the solute-solvent interaction to the solvation free energy, while it is milder for the contribution from the attractive component. Correspondingly, when the water density decreases in the interfacial region of the membrane, the reduction of the repulsive effect is stronger and the solvation free energy can be negative.
  • 83
    • 44349126423 scopus 로고    scopus 로고
    • The "excluded-volume" region can be identified over the energy coordinate as > c, where c is rather arbitrary and is typically 10-20 kcal/mol. When the integral over in Eqs. is restricted to the domain corresponding to the excluded-volume region, the integral value is larger in the order of bulk water, region IV, and region II.
    • The "excluded-volume" region can be identified over the energy coordinate as > c, where c is rather arbitrary and is typically 10-20 kcal/mol. When the integral over in Eqs. is restricted to the domain corresponding to the excluded-volume region, the integral value is larger in the order of bulk water, region IV, and region II.
  • 85
    • 44349175228 scopus 로고    scopus 로고
    • The change in the solvent-solvent interaction energy contributes to the thermodynamic enthalpy and energy. The excess partial molar enthalpy is the sum of the change in the intramolecular energy, 〈u〉, the solvent reorganization term, and the pressure-volume term (Ref.).
    • The change in the solvent-solvent interaction energy contributes to the thermodynamic enthalpy and energy. The excess partial molar enthalpy is the sum of the change in the intramolecular energy, 〈u〉, the solvent reorganization term, and the pressure-volume term (Ref.).
  • 86
    • 0003788061 scopus 로고    scopus 로고
    • 2nd ed., edited by K. S. Birdi (CRC, Boca Raton, FL).
    • Handbook of Surface and Colloid Chemistry, 2nd ed., edited by, K. S. Birdi, (CRC, Boca Raton, FL, 2003).
    • (2003) Handbook of Surface and Colloid Chemistry


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