{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,9,30]],"date-time":"2026-09-30T15:35:22Z","timestamp":1790782522449,"version":"4.1.0"},"reference-count":35,"publisher":"Springer Science and Business Media LLC","issue":"1","license":[{"start":{"date-parts":[[2014,8,18]],"date-time":"2014-08-18T00:00:00Z","timestamp":1408320000000},"content-version":"tdm","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0"},{"start":{"date-parts":[[2014,8,18]],"date-time":"2014-08-18T00:00:00Z","timestamp":1408320000000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0"}],"content-domain":{"domain":["link.springer.com"],"crossmark-restriction":false},"short-container-title":["Sci Rep"],"abstract":"<jats:title>Abstract<\/jats:title><jats:p>We report, for the first time, direct observation of coherent oscillations in the ground-state of IR775 dye due to microheterogeneous environment. Using ultrafast near-infrared degenerate pump-probe technique centered at 800\u2005nm, we present the dynamics of IR775 in a binary mixture of methanol and chloroform at ultra-short time resolution of 30\u2005fs. The dynamics of the dye in binary mixtures, in a time-scale of a few fs to ~740\u2005ps, strongly varies as a function of solvent composition (volume fraction). Multi-oscillation behavior of the coherent vibration was observed, which increased with decreasing percentage of methanol in the dye mixture. Maximum number of damped oscillations were observed in 20% methanol. The observed vibrational wavepacket motion in the ground-state is periodic in nature. We needed two cosine functions to fit the coherent oscillation data as two different solvents were used. Dynamics of the dye molecule in binary mixtures can be explained by wavepacket motion in the ground potential energy surface. More is the confinement of the dye molecule in binary mixtures, more is the number of damped oscillations. The vibrational cooling time, \u03c4<jats:sub>2<\/jats:sub>, increases with increase in the confinement of the system. The observed wavepacket oscillations in ground-state dynamics continued until 1.6\u2005ps.<\/jats:p>","DOI":"10.1038\/srep06097","type":"journal-article","created":{"date-parts":[[2014,8,18]],"date-time":"2014-08-18T09:08:58Z","timestamp":1408352938000},"update-policy":"https:\/\/doi.org\/10.1007\/springer_crossmark_policy","source":"Crossref","is-referenced-by-count":10,"title":["Direct Observation of Coherent Oscillations in Solution due to Microheterogeneous Environment"],"prefix":"10.1038","volume":"4","author":[{"given":"Dipak Kumar","family":"Das","sequence":"first","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Krishnandu","family":"Makhal","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Soumendra Nath","family":"Bandyopadhyay","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Debabrata","family":"Goswami","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"297","published-online":{"date-parts":[[2014,8,18]]},"reference":[{"key":"BFsrep06097_CR1","unstructured":"Kalyanasundaram, K. Photochemistry in Microheterogeneous Systems (Academic Press, New York, 1987)."},{"key":"BFsrep06097_CR2","doi-asserted-by":"publisher","first-page":"7312","DOI":"10.1021\/ja00414a045","volume":"103","author":"AM Braun","year":"1981","unstructured":"Braun, A. M. et al. Photochemical Processes of Benzophenone in Microheterogeneous Systems. J. Am. Chem. Soc. 103, 7312\u20137316 (1981).","journal-title":"J. Am. Chem. Soc."},{"key":"BFsrep06097_CR3","doi-asserted-by":"publisher","first-page":"424","DOI":"10.1080\/07391102.2013.773562","volume":"32","author":"PK Ghattyvenkatakrishna","year":"2014","unstructured":"Ghattyvenkatakrishna, P. K. & Carri, G. A. Effect of Glycerol-Water Binary Mixtures on the Structure and Dynamics of Protein Solutions. J. Biomol. Struct. Dyn. 32, 424\u2013437 (2014).","journal-title":"J. Biomol. Struct. Dyn."},{"key":"BFsrep06097_CR4","doi-asserted-by":"publisher","first-page":"8449","DOI":"10.1021\/jp034760i","volume":"107","author":"T Molotsky","year":"2003","unstructured":"Molotsky, T. & Huppert, D. Solvation Statics and Dynamics of Coumarin-153 in Dioxane-Water Solvent Mixtures. J. Phys. Chem. A 107, 8449\u20138457 (2003).","journal-title":"J. Phys. Chem. A"},{"key":"BFsrep06097_CR5","doi-asserted-by":"publisher","first-page":"11840","DOI":"10.1021\/jp204586p","volume":"115","author":"R Misra","year":"2011","unstructured":"Misra, R., Bhattacharyya, S. P. & Mandal, A. Spectral Response of 4-Methyl-2,6-dicarbomethoxyphenol, an Excited-State Intramolecular Proton-Transfer Probe in Cyclohexane\u2013Ethanol Mixtures: Signatures of Medium Microheterogeneity. J. Phys. Chem. B 115, 11840\u201311851 (2011).","journal-title":"J. Phys. Chem. B"},{"key":"BFsrep06097_CR6","doi-asserted-by":"publisher","first-page":"2797","DOI":"10.1021\/jz201295a","volume":"2","author":"AE Bragg","year":"2011","unstructured":"Bragg, A. E., Kanu, G. U. & Schwartz, B. J. Nanometer-Scale Phase Separation and Preferential Solvation in THF\u2013Water Mixtures: Ultrafast Electron Hydration and Recombination Dynamics Following CTTS Excitation of I\u2212. J. Phys. Chem. Lett. 2, 2797\u20132804 (2011).","journal-title":"J. Phys. Chem. Lett."},{"key":"BFsrep06097_CR7","doi-asserted-by":"publisher","first-page":"6341","DOI":"10.1021\/jp0345654","volume":"107","author":"NK Petrov","year":"2003","unstructured":"Petrov, N. K. et al. Photophysical Properties of 3,3\u2032 -Diethylthiacarbocyanine Iodide in Binary Mixtures. J. Phys. Chem. A 107, 6341\u20136350 (2003).","journal-title":"J. Phys. Chem. A"},{"key":"BFsrep06097_CR8","doi-asserted-by":"publisher","first-page":"13670","DOI":"10.1021\/jp0618680","volume":"110","author":"JL Dashnau","year":"2006","unstructured":"Dashnau, J. L., Nucci, N. V., Sharp, K. A. & Vanderkooi, J. M. Hydrogen Bonding and the Cryoprotective Properties of Glycerol\/Water Mixtures. J. Phys. Chem. B 110, 13670\u201313670 (2006).","journal-title":"J. Phys. Chem. B"},{"key":"BFsrep06097_CR9","doi-asserted-by":"publisher","first-page":"38","DOI":"10.1016\/j.cryobiol.2012.10.006","volume":"66","author":"U Ta\u015fdemir","year":"2013","unstructured":"Ta\u015fdemir, U. et al. Effects of Various Cryoprotectants on Bull Sperm Quality, DNA Integrity and Oxidative Stress Parameters. Cryobiology 66, 38\u201342 (2013).","journal-title":"Cryobiology"},{"key":"BFsrep06097_CR10","doi-asserted-by":"publisher","first-page":"813","DOI":"10.1016\/j.theriogenology.2007.06.014","volume":"68","author":"Z Rasul","year":"2007","unstructured":"Rasul, Z., Ahmed, N. & Anzar, M. Antagonist Effect of DMSO on the Cryoprotection Ability of Glycerol during Cryopreservation of Buffalo Sperm. Theriogenology 68, 813\u2013819 (2007).","journal-title":"Theriogenology"},{"key":"BFsrep06097_CR11","doi-asserted-by":"publisher","first-page":"2027","DOI":"10.1021\/jp972295h","volume":"102","author":"R Gratias","year":"1998","unstructured":"Gratias, R. & Kessler, H. Molecular-Dynamics Study on Microheterogeneity and Preferential Solvation in Methanol Chloroform Mixtures. J. Phys. Chem. B 102, 2027\u20132031 (1998).","journal-title":"J. Phys. Chem. B"},{"key":"BFsrep06097_CR12","doi-asserted-by":"publisher","first-page":"190","DOI":"10.1016\/0014-5793(92)81272-N","volume":"308","author":"KV Pervushin","year":"1992","unstructured":"Pervushin, K. V. & Arseniev, A. S. Three-Dimensional Structure of (1\u201336) Bacterioopsin in Methanol\u2014Chloroform Mixture and SDS Micelles Determined by 2D 1H-NMR Spectroscopy. FEBS 308, 190\u2013196 (1992).","journal-title":"FEBS"},{"key":"BFsrep06097_CR13","doi-asserted-by":"publisher","first-page":"665","DOI":"10.1111\/j.1432-1033.1992.tb16972.x","volume":"206","author":"IL Barsukov","year":"1992","unstructured":"Barsukov, I. L., Nolde, D. E., Lomize, A. L. & Arseniev, A. S. Three-Dimensional Structure of Proteolytic Fragment 163\u2013231 of Bacterioopsin Determined from Nuclear Magnetic Resonance Data in Solution. Eur. J. Biochem. 206, 665\u2013672 (1992).","journal-title":"Eur. J. Biochem."},{"key":"BFsrep06097_CR14","doi-asserted-by":"publisher","first-page":"223","DOI":"10.1111\/j.1432-1033.1992.tb17412.x","volume":"210","author":"VY Orekhov","year":"1992","unstructured":"Orekhov, V. Y., Abdulaeva, G. V., Musina, L. Yu. & Arseniev, A. S. 1H-15N-NMR Studies of Bacteriorhodopsin Halobacterium halobium. Eur. J. Biochem 210, 223\u2013229 (1992).","journal-title":"Eur. J. Biochem"},{"key":"BFsrep06097_CR15","doi-asserted-by":"publisher","first-page":"571","DOI":"10.1111\/j.1432-1033.1994.tb19973.x","volume":"219","author":"KV Pervushin","year":"1994","unstructured":"Pervushin, K. V. et al. Three-Dimensional Structure of (1\u201371) Bacterioopsin Solubilized in Methanol\/Chloroform and SDS Micelles Determined by 15N-1H Heteronuclear NMR Spectroscopy. Eur. J. Biochem. 219, 571\u2013583 (1994).","journal-title":"Eur. J. Biochem."},{"key":"BFsrep06097_CR16","doi-asserted-by":"publisher","first-page":"518","DOI":"10.1021\/j150551a003","volume":"61","author":"EA Moelwyn-Hughes","year":"1957","unstructured":"Moelwyn-Hughes, E. A. & Missen, R. W. Thermodynamics Properties of Methyl Alcohol-Chloromethane Solutions. J. Phys. Chem. 61, 518\u2013521 (1957).","journal-title":"J. Phys. Chem."},{"key":"BFsrep06097_CR17","doi-asserted-by":"publisher","first-page":"387","DOI":"10.1139\/v79-065","volume":"57","author":"PP Singh","year":"1979","unstructured":"Singh, P. P., Sharma, B. R. & Sidhu, K. S. Thermodynamics of Chloroform and Methanol Mixtures. Can. J. Chem. 57, 387\u2013393 (1979).","journal-title":"Can. J. Chem."},{"key":"BFsrep06097_CR18","doi-asserted-by":"publisher","first-page":"19463","DOI":"10.1021\/jp0535238","volume":"109","author":"G Kamath","year":"2005","unstructured":"Kamath, G., Georgiev, G. & Potof, J. J. Molecular Modeling of Phase Behavior and Microstructure of Acetone-Chloroform-Methanol Binary Mixtures. J. Phys. Chem. B 109, 19463\u201319473 (2005).","journal-title":"J. Phys. Chem. B"},{"key":"BFsrep06097_CR19","doi-asserted-by":"publisher","first-page":"321","DOI":"10.1103\/PhysRevLett.57.321","volume":"57","author":"MJ Rosker","year":"1986","unstructured":"Rosker, M. J., Wise, F. W. & Tang, C. L. Femtosecond Relaxation Dynamics of Large Molecules. Phys. Rev. Lett 57, 321\u2013324 (1986).","journal-title":"Phys. Rev. Lett"},{"key":"BFsrep06097_CR20","doi-asserted-by":"publisher","first-page":"1720","DOI":"10.1103\/PhysRevA.35.1720","volume":"35","author":"M Mitsunaga","year":"1987","unstructured":"Mitsunaga, M. & Tang, C. L. Theory of Quantum Beats in Optical Transmission-Correlation and Pump-Probe Measurements. Phys. Rev. A 35, 1720\u20131728 (1987).","journal-title":"Phys. Rev. A"},{"key":"BFsrep06097_CR21","doi-asserted-by":"publisher","first-page":"5761","DOI":"10.1063\/1.471337","volume":"104","author":"SH Ashworth","year":"1996","unstructured":"Ashworth, S. H. et al. Vibronic Excitations of Large Molecules in Solution Studied by Two-Color Pump\u2013Probe Experiments on the 20 fs Time Scale. J. Chem. Phys. 104, 5761\u20135769 (1996).","journal-title":"J. Chem. Phys."},{"key":"BFsrep06097_CR22","doi-asserted-by":"publisher","first-page":"12070","DOI":"10.1063\/1.479142","volume":"110","author":"T-S Yang","year":"1999","unstructured":"Yang, T.-S. et al. Femtosecond Pump-Probe Study of Molecular Vibronic Structures and Dynamics of a Cyanine Dye in Solution. J. Chem. Phys. 110, 12070\u201312081 (1999).","journal-title":"J. Chem. Phys."},{"key":"BFsrep06097_CR23","doi-asserted-by":"publisher","first-page":"2759","DOI":"10.1021\/jp980346k","volume":"102","author":"CJ Bardeen","year":"1998","unstructured":"Bardeen, C. J., Wang, Q. & Shank, C. V. Femtosecond Chirped Pulse Excitation of Vibrational Wave Packets in LD690 and Bacteriorhodopsin. J. Phys. Chem. A 102, 2759\u20132766 (1998).","journal-title":"J. Phys. Chem. A"},{"key":"BFsrep06097_CR24","doi-asserted-by":"publisher","first-page":"7546","DOI":"10.1063\/1.1313542","volume":"113","author":"K Misawa","year":"2000","unstructured":"Misawa, K. & Kobayashi, T. Wave-Packet Dynamics in a Cyanine Dye Molecule Excited with Femtosecond Chirped Pulses. J. Chem. Phys. 113, 7546\u20137553 (2000).","journal-title":"J. Chem. Phys."},{"key":"BFsrep06097_CR25","doi-asserted-by":"publisher","first-page":"101","DOI":"10.1016\/0009-2614(89)87564-5","volume":"160","author":"HL Fragnito","year":"1989","unstructured":"Fragnito, H. L., Bigot, J. -Y., Becker, P. C. & Shank, C. V. Evolution of the Vibronic Absorption Spectrum in a Molecule Following Impulsive Excitation with a 6\u2005fs Optical Pulse. Chem. Phys. Lett. 160, 101\u2013104 (1989).","journal-title":"Chem. Phys. Lett."},{"key":"BFsrep06097_CR26","doi-asserted-by":"publisher","first-page":"443","DOI":"10.1126\/science.278.5337.443","volume":"278","author":"Y Mizutani","year":"1997","unstructured":"Mizutani, Y. & Kitagawa, T. Direct Observation of Cooling of heme Upon Photodissociation of Carbonmonoxy Myoglobin. Science 278, 443\u2013446 (1997).","journal-title":"Science"},{"key":"BFsrep06097_CR27","doi-asserted-by":"publisher","first-page":"3513","DOI":"10.1039\/c2cp23167k","volume":"14","author":"O Braem","year":"2012","unstructured":"Braem, O., Penfold, T. J., Cannizzo, A. & Chergui, M. A Femtosecond Fluorescence Study of Vibrational Relaxation and Cooling Dynamics of UV Dyes. Phys. Chem. Chem. Phys. 14, 3513\u20133519 (2012).","journal-title":"Phys. Chem. Chem. Phys."},{"key":"BFsrep06097_CR28","doi-asserted-by":"publisher","first-page":"10460","DOI":"10.1021\/jp0740595","volume":"111","author":"CT Middleton","year":"2007","unstructured":"Middleton, C. T., Cohen, B. & Kohler, B. Solvent and Solvent Isotope Effects on the Vibrational Cooling Dynamics of a DNA Base Derivative. J. Phys. Chem. A 111, 10460\u201310467 (2007).","journal-title":"J. Phys. Chem. A"},{"key":"BFsrep06097_CR29","doi-asserted-by":"publisher","first-page":"6771","DOI":"10.1021\/jp4040002","volume":"117","author":"Y Zhang","year":"2013","unstructured":"Zhang, Y., Chen, J. & Kohler, B. Hydrogen Bond Donors Accelerate Vibrational Cooling of Hot Purine Derivatives in Heavy Water. J. Phys. Chem. A 117, 6771\u20136780 (2013).","journal-title":"J. Phys. Chem. A"},{"key":"BFsrep06097_CR30","doi-asserted-by":"publisher","first-page":"10370","DOI":"10.1021\/ja0161453","volume":"123","author":"J-ML Pecourt","year":"2001","unstructured":"Pecourt, J-M. L. Peon, J. & Kohler, B. DNA Excited-State Dynamics: Ultrafast Internal Conversion and Vibrational Cooling in a Series of Nucleosides. J. Am. Chem. Soc. 123, 10370\u201310378 (2001).","journal-title":"J. Am. Chem. Soc."},{"key":"BFsrep06097_CR31","doi-asserted-by":"publisher","first-page":"1197","DOI":"10.1021\/cr00014a003","volume":"92","author":"J Fabian","year":"1992","unstructured":"Fabian, J., Nakazumi, H. & Matsuoka, M. Near-Infrared Absorbing Dyes. Chem. Rev. 92, 1197\u20131226 (1992).","journal-title":"Chem. Rev."},{"key":"BFsrep06097_CR32","doi-asserted-by":"publisher","first-page":"64","DOI":"10.1016\/j.cbpa.2009.10.022","volume":"14","author":"JO Escobedo","year":"2009","unstructured":"Escobedo, J. O., Rusin, O., Lim, S. & Strongin, R. M. NIR Dyes for Bioimaging Applications. Curr. Opin. Chem. Biol. 14, 64\u201370 (2009).","journal-title":"Curr. Opin. Chem. Biol."},{"key":"BFsrep06097_CR33","doi-asserted-by":"publisher","first-page":"1329","DOI":"10.1021\/jz300363t","volume":"3","author":"A Konar","year":"2012","unstructured":"Konar, A., Shah, J. D., Lozovoy, V. V. & Dantus, M. Optical Response of Fluorescent Molecules Studied by Synthetic Femtosecond Laser Pulses. J. Phys. Chem. Lett. 3, 1329\u20131335 (2012).","journal-title":"J. Phys. Chem. Lett."},{"key":"BFsrep06097_CR34","doi-asserted-by":"publisher","first-page":"45","DOI":"10.1016\/j.cplett.2013.06.027","volume":"579","author":"DK Das","year":"2013","unstructured":"Das, D. K., Makhal, K., Singhal, S. & Goswami, D. Polarization Induced Control of Multiple Fuorescence from a Molecule. Chem. Phys. Lett. 579, 45\u201350 (2013).","journal-title":"Chem. Phys. Lett."},{"key":"BFsrep06097_CR35","doi-asserted-by":"publisher","first-page":"140","DOI":"10.1021\/je00002a003","volume":"36","author":"AM Crabtree","year":"1991","unstructured":"Crabtree, A. M. & O'Brlen, J. F. Excess Viscosities of Binary Mixtures of Chloroform and Alcohols. J. Chem. Eng. Data 36, 140\u2013142 (1991).","journal-title":"J. Chem. Eng. Data"}],"container-title":["Scientific Reports"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/www.nature.com\/articles\/srep06097","content-type":"text\/html","content-version":"vor","intended-application":"text-mining"},{"URL":"https:\/\/www.nature.com\/articles\/srep06097.pdf","content-type":"application\/pdf","content-version":"vor","intended-application":"text-mining"},{"URL":"https:\/\/www.nature.com\/articles\/srep06097.pdf","content-type":"application\/pdf","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2023,1,6]],"date-time":"2023-01-06T07:40:15Z","timestamp":1672990815000},"score":1,"resource":{"primary":{"URL":"https:\/\/www.nature.com\/articles\/srep06097"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2014,8,18]]},"references-count":35,"journal-issue":{"issue":"1","published-online":{"date-parts":[[2014,12,17]]}},"alternative-id":["BFsrep06097"],"URL":"https:\/\/doi.org\/10.1038\/srep06097","relation":{},"ISSN":["2045-2322"],"issn-type":[{"value":"2045-2322","type":"electronic"}],"subject":[],"published":{"date-parts":[[2014,8,18]]},"assertion":[{"value":"11 April 2014","order":1,"name":"received","label":"Received","group":{"name":"ArticleHistory","label":"Article History"}},{"value":"18 July 2014","order":2,"name":"accepted","label":"Accepted","group":{"name":"ArticleHistory","label":"Article History"}},{"value":"18 August 2014","order":3,"name":"first_online","label":"First Online","group":{"name":"ArticleHistory","label":"Article History"}},{"value":"The authors declare no competing financial interests.","order":1,"name":"Ethics","group":{"name":"EthicsHeading","label":"Competing interests"}}],"article-number":"6097"}}