Energetics of hydrogen bond network rearrangements in liquid water

被引:481
作者
Smith, JD [1 ]
Cappa, CD [1 ]
Wilson, KR [1 ]
Messer, BM [1 ]
Cohen, RC [1 ]
Saykally, RJ [1 ]
机构
[1] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA
关键词
D O I
10.1126/science.1102560
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
A strong temperature dependence of oxygen K-edge x-ray absorption fine structure features was observed for supercooled and normal liquid water droplets prepared from the breakup of a liquid microjet. Analysis of the data over the temperature range 251 to 288 kelvin (-22degrees to +15degreesC) yields a value of 1.5+/-0.5 kilocalories per mote for the average thermal energy required to effect an observable rearrangement between the fully coordinated ("ice-like") and distorted ("broken-donor") local hydrogen-bonding configurations responsible for the pre-edge and post-edge features, respectively. This energy equals the latent heat of melting of ice with hexagonal symmetry (ice 1=lh) and is consistent with the distribution of hydrogen bond strengths obtained for the "overstructured" ST2 model of water.
引用
收藏
页码:851 / 853
页数:3
相关论文
共 21 条
  • [1] Bergmann U, 2002, PHYS REV B, V66, DOI 10.1103/PhysRevB.66.092107
  • [2] The premelting of ice studied with photoelectron spectroscopy
    Bluhm, H
    Ogletree, DF
    Fadley, CS
    Hussain, Z
    Salmeron, N
    [J]. JOURNAL OF PHYSICS-CONDENSED MATTER, 2002, 14 (08) : L227 - L233
  • [3] CONNECTIVITY OF HYDROGEN-BONDS IN LIQUID WATER
    BLUMBERG, RL
    STANLEY, HE
    GEIGER, A
    MAUSBACH, P
    [J]. JOURNAL OF CHEMICAL PHYSICS, 1984, 80 (10) : 5230 - 5241
  • [4] X-RAY-INVESTIGATION OF SUPERCOOLED WATER
    CORBAN, R
    ZEIDLER, MD
    [J]. BERICHTE DER BUNSEN-GESELLSCHAFT-PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 1992, 96 (10): : 1463 - 1467
  • [5] LOW-DENSITY PATCHES IN THE HYDROGEN-BOND NETWORK OF LIQUID WATER - EVIDENCE FROM MOLECULAR-DYNAMICS COMPUTER-SIMULATIONS
    GEIGER, A
    STANLEY, HE
    [J]. PHYSICAL REVIEW LETTERS, 1982, 49 (24) : 1749 - 1752
  • [6] X-ray emission spectroscopy of hydrogen bonding and electronic structure of liquid water -: art. no. 137402
    Guo, JH
    Luo, Y
    Augustsson, A
    Rubensson, JE
    Såthe, C
    Ågren, H
    Siegbahn, H
    Nordgren, J
    [J]. PHYSICAL REVIEW LETTERS, 2002, 89 (13) : 137402 - 137402
  • [7] RAMAN-SPECTROSCOPIC STUDY OF DILUTE HOD IN LIQUID H2O IN THE TEMPERATURE-RANGE - 31.5 TO 160-DEGREES-C
    HARE, DE
    SORENSEN, CM
    [J]. JOURNAL OF CHEMICAL PHYSICS, 1990, 93 (10) : 6954 - 6961
  • [8] Calculation of near-edge x-ray-absorption fine structure at finite temperatures:: Spectral signatures of hydrogen bond breaking in liquid water
    Hetényi, B
    De Angelis, F
    Giannozzi, P
    Car, R
    [J]. JOURNAL OF CHEMICAL PHYSICS, 2004, 120 (18) : 8632 - 8637
  • [9] Jeffrey G.A., 1997, INTRO HYDROGEN BONDI, P11, DOI DOI 10.1246/CL.2012.65
  • [10] COMPARISON OF SIMPLE POTENTIAL FUNCTIONS FOR SIMULATING LIQUID WATER
    JORGENSEN, WL
    CHANDRASEKHAR, J
    MADURA, JD
    IMPEY, RW
    KLEIN, ML
    [J]. JOURNAL OF CHEMICAL PHYSICS, 1983, 79 (02) : 926 - 935