Real-Time Time-Frequency Two-Dimensional Imaging of Ultrafast Transient Signals in Solid-State Organic Materials

In this review, we demonstrate a real-time time-frequency two-dimensional (2D) pump-probe imaging spectroscopy implemented on a single shot basis applicable to excited-state dynamics in solid-state organic and biological materials. Using this technique, we could successfully map ultrafast time-frequency 2D transient absorption signals of β-carotene in solid films with wide temporal and spectral ranges having very short accumulation time of 20 ms per unit frame. The results obtained indicate the high potential of this technique as a powerful and unique spectroscopic tool to observe ultrafast excited-state dynamics of organic and biological materials in solid-state, which undergo rapid photodegradation.

[1]  H. S. Wolff,et al.  iRun: Horizontal and Vertical Shape of a Region-Based Graph Compression , 2022, Sensors.

[2]  K. Nelson,et al.  Dual-echelon single-shot femtosecond spectroscopy. , 2000, Optics letters.

[3]  K. Nelson,et al.  Pulse-length-limited ultrafast pump-probe spectroscopy in a single laser shot. , 1994, Optics Letters.

[4]  G. Lewis,et al.  The Color of Organic Substances. , 1939 .

[5]  H. Hashimoto,et al.  Ultrafast dynamics of all-trans--carotene explored by resonant and nonresonant photoexcitations. , 2005, Physical review letters.

[6]  H. Frank,et al.  Effect of isomer geometry on the steady-state absorption spectra and femtosecond time-resolved dynamics of carotenoids. , 2005, The journal of physical chemistry. B.

[7]  G. Cerullo,et al.  Photosynthetic Light Harvesting by Carotenoids: Detection of an Intermediate Excited State , 2002, Science.

[8]  J. G. Victor,et al.  On measuring the distribution of local free volume in glassy polymers by photochromic and fluorescence techniques , 1987 .

[9]  Takayoshi Kobayashi,et al.  Sequential singlet internal conversion of 1Bu+ → 3Ag− → 1Bu− → 2Ag− → (1Ag− ground) in all-trans-spirilloxanthin revealed by two-dimensional sub-5-fs spectroscopy , 2004 .

[10]  J. Takeda,et al.  Femtosecond Real-Time Pump-Probe Imaging Spectroscopy Implemented on a Single Shot Basis , 2006 .

[11]  M. Kimura,et al.  Time–frequency two-dimensional mapping of rapid energy transfer in light-harvesting star-shaped dendrimers , 2008 .

[12]  See Leang Chin,et al.  BAND-GAP DEPENDENCE OF THE ULTRAFAST WHITE-LIGHT CONTINUUM , 1998 .

[13]  V. Sundström,et al.  Ultrafast dynamics of carotenoid excited States-from solution to natural and artificial systems. , 2004, Chemical reviews.

[14]  G. Lanzani,et al.  Conjugation length dependence of internal conversion in carotenoids: role of the intermediate state. , 2004, Physical review letters.

[15]  H. Hashimoto,et al.  Vibrational relaxation of the 2 A g − excited state in all- trans -β-carotene obtained by femtosecond time-resolved Raman spectroscopy , 2001 .

[16]  T. Tahara,et al.  Time-wavelength two-dimensional femtosecond fluorescence imaging. , 2004, Optics letters.

[17]  Jianping Zhang,et al.  Vibronic Coupling through the In-Phase, CC Stretching Mode Plays a Major Role in the 2Ag- to 1Ag- Internal Conversion of all-trans-β-Carotene , 2000 .

[18]  J. Takeda,et al.  Direct visualization of transient absorption by real-time pump-probe imaging spectroscopy , 2005 .

[19]  Jun Takeda,et al.  Femtosecond real-time pump-probe imaging spectroscopy , 2004 .

[20]  Delmar S. Larsen,et al.  Excited state dynamics of β-carotene explored with dispersed multi-pulse transient absorption , 2003 .

[21]  R. Cogdell,et al.  Carotenoids in Photosynthesis , 1996, Photochemistry and photobiology.

[22]  Minoru Obara,et al.  Generation and characterization of ultrafast white-light continuum in condensed media. , 2002, Applied optics.

[23]  M. Kimura,et al.  Rapid energy transfer in a dendrimer having π-conjugated light-harvesting antennas , 2008 .

[24]  N. Sugimoto,et al.  Efficient optical Kerr shutter for femtosecond time-resolved luminescence spectroscopy , 2000 .

[25]  L. Skibsted,et al.  The 1Bu-type singlet state of β-carotene as a precursor of the radical cation found in chloroform solution by sub-picosecond time-resolved absorption spectroscopy , 2001 .

[26]  R. Cogdell,et al.  Pump-deplete-probe spectroscopy and the puzzle of carotenoid dark states , 2004 .

[27]  K. Nelson,et al.  Irreversible Organic Crystalline Chemistry Monitored in Real Time , 2006, Science.

[28]  Inter-molecular interaction of photochromic furylfulgide dispersed in a polymer film , 1992 .

[29]  Tohru Suemoto,et al.  Femtosecond optical Kerr gate fluorescence spectroscopy for ultrafast relaxation processes , 2000 .

[30]  L. N. Ferguson.  Relationships between Absorption Spectra and Spectra and Chemical Constitution of Organic Molecules. , 1948 .

[31]  Rick Trebino,et al.  Spatially encoded, single-shot ultrafast spectroscopies , 1995 .

[32]  K. Nakajima,et al.  Time-resolved luminescence spectroscopy by the optical Kerr-gate method applicable to ultrafast relaxation processes , 2000 .

[33]  T. Gillbro,et al.  Solvent Dependence of the Ultrafast S2−S1 Internal Conversion Rate of β-Carotene , 1998 .

[34]  M. Maroncelli,et al.  Design and Characterization of a Femtosecond Fluorescence Spectrometer Based on Optical Kerr Gating , 2005, Applied spectroscopy.

[35]  H. Hashimoto,et al.  Excitation energy dependence of excited states dynamics in all-trans-carotenes determined by femtosecond absorption and fluorescence spectroscopy , 2005 .