DOI: 10.1063/1.453507. Time-resolved fluorescence and hole-burning line shapes of solvated molecules: Longitudinal dielectric relaxation and vibrational dynamics

Time-resolved fluorescence and hole-burning line shapes of solvated molecules: Longitudinal dielectric relaxation and vibrational dynamics

10.1063/1.453507

Crossref journal-article

AIP Publishing

The Journal of Chemical Physics (317)

Abstract

We develop a microscopic theory of time- and frequency-resolved fluorescence and hole-burning measurements of polar, polyatomic molecules in a polar solvent. The line shapes are expressed in terms of gas phase spectroscopic parameters of the solute, vibrational relaxation rates, laser pulse shapes, and the dynamics of a solvation coordinate. These dynamics are then related to the frequency and wave vector dependent dielectric function of the solvent. Both fluorescence and hole-burning line shapes are predicted to show significant line narrowing at short times, and to undergo broadening and a red shift as the solvent relaxes. We propose hole burning as an alternative to fluorescence measurements in probing solvation dynamics. The time scale of the solvent induced line shift and line broadening is found to be independent of the shape of the solute, in contrast with previous work. The effects of vibrational relaxation are distinguished from those of solvent relaxation.

Bibliography

Loring, R. F., Yan, Y. J., & Mukamel, S. (1987). Time-resolved fluorescence and hole-burning line shapes of solvated molecules: Longitudinal dielectric relaxation and vibrational dynamics. The Journal of Chemical Physics, 87(10), 5840â5857.

Authors 3

Roger F. Loring (first)
Yi Jing Yan (additional)
Shaul Mukamel (additional)

References 43 Referenced 188

{'key': '2024021005362541100_r1'}
{'key': '2024021005362541100_r2'}
10.1246/bcsj.36.654 / Bull. Chem. Soc. Jpn. (1963)
{'key': '2024021005362541100_r4', 'first-page': '446', 'volume': '16', 'year': '1964', 'journal-title': 'Opt. Spectrosc.'} / Opt. Spectrosc. (1964)
10.1143/JPSJ.9.594 / J. Phys. Soc. Jpn. (1954)
10.1021/j150521a017 / J. Phys. Chem. (1954)
10.1021/ja01299a050 / J. Am. Chem. Soc. (1936)
10.1021/j100511a014 / J. Phys. Chem. (1978)
{'key': '2024021005362541100_r9', 'first-page': '417', 'volume': '44', 'year': '1977', 'journal-title': 'Opt. Spectrosc.'} / Opt. Spectrosc. (1977)
10.1016/0009-2614(83)87101-2 / Chem. Phys. Lett. (1983)
10.1021/j100295a008 / J. Phys. Chem. (1987)
10.1063/1.452249 / J. Chem. Phys. (1987)
10.1063/1.452460 / J. Chem. Phys. (1987)
10.1063/1.452029 / J. Chem. Phys. (1987)
{'key': '2024021005362541100_r13', 'first-page': '490', 'volume': '28', 'year': '1970', 'journal-title': 'Opt. Spectrosc.'} / Opt. Spectrosc. (1970)
10.1016/0301-0104(84)80014-2 / Chem. Phys. (1984)
10.1021/j100266a008 / J. Phys. Chem. (1985)
10.1016/0009-2614(87)87210-X / Chem. Phys. Lett. (1987)
10.1021/j100290a007 / J. Phys. Chem. (1987)
10.1080/00268977500100341 / Mol. Phys. (1975)
10.1021/j100218a031 / J. Phys. Chem. (1982)
{'key': '2024021005362541100_r18a'}
10.1063/1.453311 / J. Chem. Phys. (1987)
{'key': '2024021005362541100_r20'}
{'key': '2024021005362541100_r20a'}
10.1016/0030-4018(76)90067-5 / Opt. Commun. (1976)
10.1063/1.1743326 / J. Chem. Phys. (1957)
{'key': '2024021005362541100_r23'}
{'key': '2024021005362541100_r24'}
10.1063/1.446084 / J. Chem. Phys. (1983)
10.1021/j100299a005 / J. Phys. Chem. (1987)
10.1063/1.1733886 / J. Chem. Phys. (1963)
10.1063/1.1696913 / J. Chem. Phys. (1965)
{'key': '2024021005362541100_r28'}
{'key': '2024021005362541100_r29', 'first-page': '388', 'volume': '48', 'year': '1980', 'journal-title': 'Opt. Spectrosc.'} / Opt. Spectrosc. (1980)
10.1063/1.444510 / J. Chem. Phys. (1983)
10.1063/1.451502 / J. Chem. Phys. (1986)
10.1063/1.453177 / J. Chem. Phys. (1987)
10.1063/1.445807 / J. Chem. Phys. (1983)
{'key': '2024021005362541100_r33', 'first-page': '595', 'volume': '4', 'year': '1986', 'journal-title': 'J. Opt. Soc. Am. B'} / J. Opt. Soc. Am. B (1986)
10.1016/0009-2614(85)85113-7 / Chem. Phys. Lett. (1985)
10.1103/PhysRevA.33.1099 / Phys. Rev. A (1986)
10.1063/1.450515 / J. Chem. Phys. (1986)

Dates

Type	When
Created	23 years ago (July 26, 2002, 9:20 a.m.)
Deposited	1 year, 6 months ago (Feb. 10, 2024, 2:10 a.m.)
Indexed	1 year, 6 months ago (Feb. 11, 2024, 8:02 a.m.)
Issued	37 years, 9 months ago (Nov. 15, 1987)
Published	37 years, 9 months ago (Nov. 15, 1987)
Published Print	37 years, 9 months ago (Nov. 15, 1987)

Funders 0

None

BibTeX

@article{Loring_1987, title={Time-resolved fluorescence and hole-burning line shapes of solvated molecules: Longitudinal dielectric relaxation and vibrational dynamics}, volume={87}, ISSN={1089-7690}, url={http://dx.doi.org/10.1063/1.453507}, DOI={10.1063/1.453507}, number={10}, journal={The Journal of Chemical Physics}, publisher={AIP Publishing}, author={Loring, Roger F. and Yan, Yi Jing and Mukamel, Shaul}, year={1987}, month=nov, pages={5840–5857} }

JSON

{
  "indexed": {
    "date-parts": [
      [
        2024,
        2,
        11
      ]
    ],
    "date-time": "2024-02-11T13:02:53Z",
    "timestamp": 1707656573950
  },
  "reference-count": 43,
  "publisher": "AIP Publishing",
  "issue": "10",
  "content-domain": {
    "domain": [
      "pubs.aip.org"
    ],
    "crossmark-restriction": true
  },
  "published-print": {
    "date-parts": [
      [
        1987,
        11,
        15
      ]
    ]
  },
  "abstract": "<jats:p>We develop a microscopic theory of time- and frequency-resolved fluorescence and hole-burning measurements of polar, polyatomic molecules in a polar solvent. The line shapes are expressed in terms of gas phase spectroscopic parameters of the solute, vibrational relaxation rates, laser pulse shapes, and the dynamics of a solvation coordinate. These dynamics are then related to the frequency and wave vector dependent dielectric function of the solvent. Both fluorescence and hole-burning line shapes are predicted to show significant line narrowing at short times, and to undergo broadening and a red shift as the solvent relaxes. We propose hole burning as an alternative to fluorescence measurements in probing solvation dynamics. The time scale of the solvent induced line shift and line broadening is found to be independent of the shape of the solute, in contrast with previous work. The effects of vibrational relaxation are distinguished from those of solvent relaxation.</jats:p>",
  "DOI": "10.1063/1.453507",
  "type": "journal-article",
  "created": {
    "date-parts": [
      [
        2002,
        7,
        26
      ]
    ],
    "date-time": "2002-07-26T13:20:05Z",
    "timestamp": 1027689605000
  },
  "page": "5840-5857",
  "update-policy": "http://dx.doi.org/10.1063/aip-crossmark-policy-page",
  "source": "Crossref",
  "is-referenced-by-count": 188,
  "title": "Time-resolved fluorescence and hole-burning line shapes of solvated molecules: Longitudinal dielectric relaxation and vibrational dynamics",
  "prefix": "10.1063",
  "volume": "87",
  "author": [
    {
      "given": "Roger F.",
      "family": "Loring",
      "sequence": "first",
      "affiliation": [
        {
          "name": "Department of Chemistry, University of Rochester, Rochester, New York 14627"
        }
      ]
    },
    {
      "given": "Yi Jing",
      "family": "Yan",
      "sequence": "additional",
      "affiliation": [
        {
          "name": "Department of Chemistry, University of Rochester, Rochester, New York 14627"
        }
      ]
    },
    {
      "given": "Shaul",
      "family": "Mukamel",
      "sequence": "additional",
      "affiliation": [
        {
          "name": "Department of Chemistry, University of Rochester, Rochester, New York 14627"
        }
      ]
    }
  ],
  "member": "317",
  "reference": [
    {
      "key": "2024021005362541100_r1"
    },
    {
      "key": "2024021005362541100_r2"
    },
    {
      "key": "2024021005362541100_r3",
      "doi-asserted-by": "crossref",
      "first-page": "654",
      "DOI": "10.1246/bcsj.36.654",
      "volume": "36",
      "year": "1963",
      "journal-title": "Bull. Chem. Soc. Jpn."
    },
    {
      "key": "2024021005362541100_r4",
      "first-page": "446",
      "volume": "16",
      "year": "1964",
      "journal-title": "Opt. Spectrosc."
    },
    {
      "key": "2024021005362541100_r5",
      "doi-asserted-by": "crossref",
      "first-page": "594",
      "DOI": "10.1143/JPSJ.9.594",
      "volume": "9",
      "year": "1954",
      "journal-title": "J. Phys. Soc. Jpn."
    },
    {
      "key": "2024021005362541100_r6",
      "doi-asserted-by": "crossref",
      "first-page": "1002",
      "DOI": "10.1021/j150521a017",
      "volume": "58",
      "year": "1954",
      "journal-title": "J. Phys. Chem."
    },
    {
      "key": "2024021005362541100_r7",
      "doi-asserted-by": "crossref",
      "first-page": "1486",
      "DOI": "10.1021/ja01299a050",
      "volume": "58",
      "year": "1936",
      "journal-title": "J. Am. Chem. Soc."
    },
    {
      "key": "2024021005362541100_r8",
      "doi-asserted-by": "crossref",
      "first-page": "2415",
      "DOI": "10.1021/j100511a014",
      "volume": "82",
      "year": "1978",
      "journal-title": "J. Phys. Chem."
    },
    {
      "key": "2024021005362541100_r9",
      "first-page": "417",
      "volume": "44",
      "year": "1977",
      "journal-title": "Opt. Spectrosc."
    },
    {
      "key": "2024021005362541100_r9a",
      "doi-asserted-by": "crossref",
      "first-page": "339",
      "DOI": "10.1016/0009-2614(83)87101-2",
      "volume": "94",
      "year": "1983",
      "journal-title": "Chem. Phys. Lett."
    },
    {
      "key": "2024021005362541100_r10",
      "doi-asserted-by": "crossref",
      "first-page": "2693",
      "DOI": "10.1021/j100295a008",
      "volume": "91",
      "year": "1987",
      "journal-title": "J. Phys. Chem."
    },
    {
      "key": "2024021005362541100_r11",
      "doi-asserted-by": "crossref",
      "first-page": "1090",
      "DOI": "10.1063/1.452249",
      "volume": "86",
      "year": "1987",
      "journal-title": "J. Chem. Phys."
    },
    {
      "key": "2024021005362541100_r11a",
      "doi-asserted-by": "crossref",
      "first-page": "6221",
      "DOI": "10.1063/1.452460",
      "volume": "86",
      "year": "1987",
      "journal-title": "J. Chem. Phys."
    },
    {
      "key": "2024021005362541100_r12",
      "doi-asserted-by": "crossref",
      "first-page": "3183",
      "DOI": "10.1063/1.452029",
      "volume": "86",
      "year": "1987",
      "journal-title": "J. Chem. Phys."
    },
    {
      "key": "2024021005362541100_r13",
      "first-page": "490",
      "volume": "28",
      "year": "1970",
      "journal-title": "Opt. Spectrosc."
    },
    {
      "key": "2024021005362541100_r14",
      "doi-asserted-by": "crossref",
      "first-page": "257",
      "DOI": "10.1016/0301-0104(84)80014-2",
      "volume": "86",
      "year": "1984",
      "journal-title": "Chem. Phys."
    },
    {
      "key": "2024021005362541100_r15",
      "doi-asserted-by": "crossref",
      "first-page": "4181",
      "DOI": "10.1021/j100266a008",
      "volume": "89",
      "year": "1985",
      "journal-title": "J. Phys. Chem."
    },
    {
      "key": "2024021005362541100_r16",
      "doi-asserted-by": "crossref",
      "first-page": "23",
      "DOI": "10.1016/0009-2614(87)87210-X",
      "volume": "135",
      "year": "1987",
      "journal-title": "Chem. Phys. Lett."
    },
    {
      "key": "2024021005362541100_r16a",
      "doi-asserted-by": "crossref",
      "first-page": "1302",
      "DOI": "10.1021/j100290a007",
      "volume": "91",
      "year": "1987",
      "journal-title": "J. Phys. Chem."
    },
    {
      "key": "2024021005362541100_r17",
      "doi-asserted-by": "crossref",
      "first-page": "405",
      "DOI": "10.1080/00268977500100341",
      "volume": "29",
      "year": "1975",
      "journal-title": "Mol. Phys."
    },
    {
      "key": "2024021005362541100_r18",
      "doi-asserted-by": "crossref",
      "first-page": "4244",
      "DOI": "10.1021/j100218a031",
      "volume": "86",
      "year": "1982",
      "journal-title": "J. Phys. Chem."
    },
    {
      "key": "2024021005362541100_r18a"
    },
    {
      "key": "2024021005362541100_r19",
      "doi-asserted-by": "crossref",
      "first-page": "1272",
      "DOI": "10.1063/1.453311",
      "volume": "87",
      "year": "1987",
      "journal-title": "J. Chem. Phys."
    },
    {
      "key": "2024021005362541100_r20"
    },
    {
      "key": "2024021005362541100_r20a"
    },
    {
      "key": "2024021005362541100_r21",
      "doi-asserted-by": "crossref",
      "first-page": "128",
      "DOI": "10.1016/0030-4018(76)90067-5",
      "volume": "16",
      "year": "1976",
      "journal-title": "Opt. Commun."
    },
    {
      "key": "2024021005362541100_r22",
      "doi-asserted-by": "crossref",
      "first-page": "454",
      "DOI": "10.1063/1.1743326",
      "volume": "26",
      "year": "1957",
      "journal-title": "J. Chem. Phys."
    },
    {
      "key": "2024021005362541100_r23"
    },
    {
      "key": "2024021005362541100_r24"
    },
    {
      "key": "2024021005362541100_r25",
      "doi-asserted-by": "crossref",
      "first-page": "2126",
      "DOI": "10.1063/1.446084",
      "volume": "79",
      "year": "1983",
      "journal-title": "J. Chem. Phys."
    },
    {
      "key": "2024021005362541100_r26",
      "doi-asserted-by": "crossref",
      "first-page": "3938",
      "DOI": "10.1021/j100299a005",
      "volume": "91",
      "year": "1987",
      "journal-title": "J. Phys. Chem."
    },
    {
      "key": "2024021005362541100_r27",
      "doi-asserted-by": "crossref",
      "first-page": "1858",
      "DOI": "10.1063/1.1733886",
      "volume": "38",
      "year": "1963",
      "journal-title": "J. Chem. Phys."
    },
    {
      "key": "2024021005362541100_r27a",
      "doi-asserted-by": "crossref",
      "first-page": "1261",
      "DOI": "10.1063/1.1696913",
      "volume": "43",
      "year": "1965",
      "journal-title": "J. Chem. Phys."
    },
    {
      "key": "2024021005362541100_r28"
    },
    {
      "key": "2024021005362541100_r29",
      "first-page": "388",
      "volume": "48",
      "year": "1980",
      "journal-title": "Opt. Spectrosc."
    },
    {
      "key": "2024021005362541100_r30",
      "doi-asserted-by": "crossref",
      "first-page": "365",
      "DOI": "10.1063/1.444510",
      "volume": "78",
      "year": "1983",
      "journal-title": "J. Chem. Phys."
    },
    {
      "key": "2024021005362541100_r31",
      "doi-asserted-by": "crossref",
      "first-page": "5908",
      "DOI": "10.1063/1.451502",
      "volume": "85",
      "year": "1986",
      "journal-title": "J. Chem. Phys."
    },
    {
      "key": "2024021005362541100_r31a",
      "doi-asserted-by": "crossref",
      "first-page": "2021",
      "DOI": "10.1063/1.453177",
      "volume": "87",
      "year": "1987",
      "journal-title": "J. Chem. Phys."
    },
    {
      "key": "2024021005362541100_r32",
      "doi-asserted-by": "crossref",
      "first-page": "603",
      "DOI": "10.1063/1.445807",
      "volume": "79",
      "year": "1983",
      "journal-title": "J. Chem. Phys."
    },
    {
      "key": "2024021005362541100_r33",
      "first-page": "595",
      "volume": "4",
      "year": "1986",
      "journal-title": "J. Opt. Soc. Am. B"
    },
    {
      "key": "2024021005362541100_r34",
      "doi-asserted-by": "crossref",
      "first-page": "426",
      "DOI": "10.1016/0009-2614(85)85113-7",
      "volume": "114",
      "year": "1985",
      "journal-title": "Chem. Phys. Lett."
    },
    {
      "key": "2024021005362541100_r34a",
      "doi-asserted-by": "crossref",
      "first-page": "1099",
      "DOI": "10.1103/PhysRevA.33.1099",
      "volume": "33",
      "year": "1986",
      "journal-title": "Phys. Rev. A"
    },
    {
      "key": "2024021005362541100_r35",
      "doi-asserted-by": "crossref",
      "first-page": "1228",
      "DOI": "10.1063/1.450515",
      "volume": "84",
      "year": "1986",
      "journal-title": "J. Chem. Phys."
    }
  ],
  "container-title": "The Journal of Chemical Physics",
  "original-title": [],
  "language": "en",
  "link": [
    {
      "URL": "https://pubs.aip.org/aip/jcp/article-pdf/87/10/5840/18968039/5840_1_online.pdf",
      "content-type": "application/pdf",
      "content-version": "vor",
      "intended-application": "syndication"
    },
    {
      "URL": "https://pubs.aip.org/aip/jcp/article-pdf/87/10/5840/18968039/5840_1_online.pdf",
      "content-type": "unspecified",
      "content-version": "vor",
      "intended-application": "similarity-checking"
    }
  ],
  "deposited": {
    "date-parts": [
      [
        2024,
        2,
        10
      ]
    ],
    "date-time": "2024-02-10T07:10:20Z",
    "timestamp": 1707549020000
  },
  "score": 1,
  "resource": {
    "primary": {
      "URL": "https://pubs.aip.org/jcp/article/87/10/5840/94030/Time-resolved-fluorescence-and-hole-burning-line"
    }
  },
  "subtitle": [],
  "short-title": [],
  "issued": {
    "date-parts": [
      [
        1987,
        11,
        15
      ]
    ]
  },
  "references-count": 43,
  "journal-issue": {
    "issue": "10",
    "published-print": {
      "date-parts": [
        [
          1987,
          11,
          15
        ]
      ]
    }
  },
  "URL": "http://dx.doi.org/10.1063/1.453507",
  "relation": {},
  "ISSN": [
    "0021-9606",
    "1089-7690"
  ],
  "subject": [],
  "published-other": {
    "date-parts": [
      [
        1987,
        11,
        15
      ]
    ]
  },
  "published": {
    "date-parts": [
      [
        1987,
        11,
        15
      ]
    ]
  }
}