Authorship：Corresponding author   Publishing type：Research paper (scientific journal)   Publisher：{AIP} Publishing  

DOI： 10.1063/1.4907530

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Publishing type：Research paper (scientific journal)  

DOI： 10.1103/PhysRevLett.92.145503

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：AMER ASSOC ADVANCEMENT SCIENCE  

High-resolution infrared and microwave spectra of He-N-carbonyl sulfide (He-N-OCS) clusters with N ranging from 2 to 8 have been detected and unambiguously assigned. The spectra show the formation of a solvation layer beginning with an equatorial "donut" of five helium atoms around the OCS molecule. The cluster moment of inertia increases as a function of N and overshoots the liquid droplet limit for N > 5, implying that even atoms in the first solvation shell are decoupled from the OCS rotation in helium nanodroplets. To the extent that this is due to superfluidity, the results directly explore the microscopic evolution of a phenomenon that is formally macroscopic in nature.

DOI： 10.1126/science.1073718

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Publishing type：Research paper (scientific journal)  

DOI： 10.1086/320469

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DOI： 10.1126/science.284.5411.135

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：EDP Sciences  

We report the first laboratory and interstellar detection of the α-cyano vinyl radical (H₂CCCN). This species was produced in the laboratory by an electric discharge of a gas mixture of vinyl cyanide, CH₂CHCN, and Ne. Its rotational spectrum was characterized using a Balle-Flygare narrowband-type Fourier-transform microwave spectrometer operating in the frequency region of 8–40 GHz. The observed spectrum shows a complex structure due to tunneling splittings between two torsional sublevels of the ground vibronic state, 0⁺ and 0⁻, derived from a large-amplitude inversion motion. In addition, the presence of two equivalent hydrogen nuclei makes it necessary to discern between ortho- and para-H₂CCCN. A least-squares analysis reproduces the observed transition frequencies with a standard deviation of ca. 3 kHz. Using the laboratory predictions, this radical was detected in the cold dark cloud TMC-1 using the Yebes 40 m telescope and the QUIJOTE¹ line survey. The 4_0, 4-3_0, 3 and 5_0, 5-4_0, 4 rotational transitions, composed of several hyperfine components, were observed in the 31.0–50.4 GHz range. Adopting a rotational temperature of 6 K, we derived a column density of (1.4±0.2)×10¹¹ cm⁻² and (1.1±0.2)×10¹¹ cm⁻² for ortho-H₂CCCN and para-H₂CCCN, respectively. The reaction of C + CH₃CN emerges as the most likely route to H₂CCCN in TMC-1, and possibly that of N + CH₂CCH as well.

DOI： 10.1051/0004-6361/202347385

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

A Fourier-transform microwave spectrum of the cis-β-cyanovinyl radical is re-measured for the K_a = 0 ladder of the a-type transitions up to 30 GHz and the 2₁₂–1₁₁ transition at 19.85 GHz.

DOI： 10.1039/d2cp00516f

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Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.jms.2022.111594

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Publishing type：Research paper (scientific journal)   Publisher：Elsevier {BV}  

DOI： 10.1016/j.jms.2018.01.007

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：ACADEMIC PRESS INC ELSEVIER SCIENCE  

The present paper reports high-resolution spectroscopic study of the (HO3)-H-14 radical in the 2000-3000 cm(-1) region, where eight E'-A'(2) bands from the ground state are observed. Three bands at 2206, 2246, and 2377 cm(-1) are analyzed for the first time, and assigned to the v(1) + 3v(4), 2v(2) + 2v(4), and v(3) + 3v(4) bands, respectively. Bands at 2024, 2155, 2518, and 2585 cm(-1) are reassigned to the vi + v(3), 2v(3), v(1) + v(3) + 7(4), and 2v(3) + v(4) bands, respectively, by adopting the new v(3) vibrational frequency of 1055 cm(-1) lower than the previous v(3) = 1492 cm(-1). The band at 2902 cm(-1) is observed for the first time and assigned to the + v(3) + 2v(4) band which is the v(1) combined band with the 1927 cm(-1) band. Band intensities observed in the 2000-3000 cm(-1) region are attributed to the intensity borrowing from the (B) over tilde E-2'-(X) over tilde (2)/1'2 electronic transition through the vibronic interaction. Although the v(3) fundamental band has not been observed due to the cancelation of vibrational intensity and borrowed intensity, the 2v(3) band becomes stronger than v(3) by a factor of more than 50. Perturbation effects are recognized for the bands observed except for the 2206 cm(-1) and 2377 cm(-1) bands, and are analyzed by taking into account the Coriolis interaction in the most cases. However, the 2024 cm(-1) band is free from the Coriolis interaction, and the v(1)-v(3) interaction is incorporated in the analysis, leading to the 2v(1) frequency of 2008.8 cm(-1), which is close to the energy value of 2010 cm(-1) observed by a laser induced fluorescence study. (C) 2017 Elsevier Inc. All rights reserved.

DOI： 10.1016/jjms.2017.09.012

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Astronomical Society  

DOI： 10.3847/0004-637x/822/2/115

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Other Link： http://stacks.iop.org/0004-637X/822/i=2/a=115?key=crossref.ebb7e4467a0a0a6600394e2fa845eca1

Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Institute of Physics Inc.  

DOI： 10.1063/1.4943286

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：ACADEMIC PRESS INC ELSEVIER SCIENCE  

The vibration-rotational structure of the ground A(2)', state of the NO3 radical is re-considered, because Hirota (2015) presented an objection to the vibrational assignment of our previous papers (Kawaguchi et al., 2011, 2013; Fujimori et al., 2013). The present study examines the vibrational assignment in the following points, (1) laser induced fluorescence (LIF) spectra observed by Fukushima and Ishiwata in the 1050 cm(-1) region, (2) Fourier transform (FT) spectra of vibrational bands from the v(4) = 1 state, and a diode laser spectrum of the 2v(4) band. These considerations support our previous assignments, that is, v(3) + v(4)= 1492 cm(-1) and v(3) = 1055 cm(-1) for (NO3)-N-14. (C) 2015 Elsevier Inc. All rights reserved.

DOI： 10.1016/j.jms.2015.06.008

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：ELSEVIER SCIENCE BV  

A cw-OPO laser system has been used to measure pressure broadening coefficients for the v(4) vibration-rotation transitions of CH3F by using Stark modulated Lamb dips. Eight pressure coefficients were determined from various pressure data, where each line shape was fitted to the Lorentzian function. The (r)Q(1,0) coefficient was found to be largely different from that of R-r(0,0), where the upper states of both transitions have the same J and K values but different parities of the l-type doublet. The coefficient for (r)Q(7,4) obtained in the present study agrees with that obtained by a Voigt profile analysis (Cartlidge and Butcher, 1990). (C) 2014 Elsevier B.V. All rights reserved.

DOI： 10.1016/j.cplett.2014.11.040

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：AMER CHEMICAL SOC  

High-resolution Fourier transform infrared spectra of the (NO3)-N-15 v(3)+v(4) and v(3)+v(4) v(4) bands were observed in the 1472 and 1112 cm(-1) regions. Compared with the case of N-14 species, large effects of perturbations were recognized in many rotational levels of the (NO3)-N-15 v(3)+v(4) state, and it was found that the v(2)+2v(4) state is responsible for the perturbation. Although a direct Coriolis interaction (Delta v(2) = 1, Delta v(3)(or Delta v(4))=1) is not present between these two vibrational levels, anharmonic terms including Phi 344 and Phi 444 mix v(3)+v(4) and 3v(4),v(2)+2v(4), v(2)+2v(4), and v(2)+2v(4) mixes with v(2)+v(4) to produce Coriolis interaction between v(3)+v(4) and v(2)+2v(4). An analysis gave the energy difference of 7.274 cm(-1) between two levels, and interaction parameters were determined. Similar perturbation analysis was applied for the 14N species, and the previous P-P(N,K) assignment of the v(3)+v(4) A'-v(4) E' band was changed for giving one A(2)', state. Spectral lines to another A,' state were not assigned because of weak intensity, which is explained by intensity anomaly through vibronic interaction, reflecting the transition moment of the (B) over tilde E-2'-(X) over tildeA'2. electronic band.

DOI： 10.1021/jp407822g

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：AMER INST PHYSICS  

The coherence decay of the v = 2 vibrational state (vibrons) of solid parahydrogen was measured via time-resolved coherent anti-Stokes Raman spectroscopy. We found that the decay curve has a non-exponential time profile in the time scale of 200 ns at a low temperature below 5 K and a low orthohydrogen impurity concentration (similar to 0.01%). This behavior, as also observed in the case of the v = 1 vibrons, represents a signature of band structure of the v = 2 state in the solid phase. The maximum coherence decay time of 50 ns in an exponential part was achieved, which shows excellence of the v = 2 state for coherent processes. We also found that finite temperatures, orthohydrogen impurities, and other structural inhomogeneity accelerate the decay, hiding the non-exponential feature of the vibron band. (C) 2013 American Institute of Physics. [http://dx.doi.org/10.1063/1.4773893]

DOI： 10.1063/1.4773893

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DOI： 10.1016/j.jms.2012.11.005

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DOI： 10.1140/epjd/e2012-30529-x

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DOI： 10.1063/1.4808035

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：AMER CHEMICAL SOC  

We report measurements of FT-IR absorption spectroscopy of HF, DF, and their clusters in solid parahydrogen (pH(2)). The observed spectra contain many absorption lines which were assigned to HF monomers, HF polymers, and clusters with other species, such as N-2, O-2, orthohydrogen (oH(2)), etc. The rotational constants of HF and DF monomers were determined from the cooperative transitions of the vibration of solid pH(2) and the rotation of HF and DF. Small reduction of the rotational constants indicates that HF and DF are nearly free rotors in solid pH(2). Time dependence of the spectra suggests that HF and DF monomers migrate in solid pH(2) and form larger polymers, probably via tunneling reactions through high energy barriers on inserting another monomer to the polymers. The line width of HF monomers in solid pH(2) was found to be 4 cm(-1), which is larger than that of other hydrogen halides in solid pH(2). This broad line width is explained by rapid rotational relaxation due to the accidental coincidence between the rotational energy of HF and the phonon energy with maximum density of states of solid pH(2) and the rotational translational coupling in a trapping site.

DOI： 10.1021/jp207419m

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：ACADEMIC PRESS INC ELSEVIER SCIENCE  

We report the infrared spectrum of NO3 studied with a high-resolution Fourier transform spectrometer. By improving the setup of an absorption cell, the following eight bands were observed at 1127, 1132, 1134, 1173, 1413, 1492, 1562, 1927 cm(-1) in the 1000-1930 cm(-1) region. The 1127, 1132, 1134, and 1562 bands were not reported previously by matrix isolation spectroscopy, and these bands have been assigned to hot bands from the v(4) state (v(3) + v(4) <- v(4)) and (v(3) + 2v(4) <- v(4)). The analysis of the 1127 band with an E'-E' type spectral pattern has been carried out, and major molecular constants of the lower (v(4)) state are determined as follows: B = 0.459 2222(60), C = 0.227 8233(40), C zeta(4) = -0.042 063(15). and v(4) = 365.48419(43) cm(-1). Two A'-E' type bands with band origin frequencies of 1132 and 1134 cm(-1) are also assigned, indicating that the 1492 band is assignable to v(3) + v(4), in contrast to the previous v(3) assignment. A simultaneous analysis of the 1127, 1132, 1134, 1492 cm(-1) bands has been carried out to give 46 molecular constants for the v(3) + v(4) and v(4) states. The molecular constants of the v(3) + v(4) A' states are different from those of the E' state, because of an effect of vibronic interaction from the (B) over tilde E-2' electronic state to the v(3) + v(4) E' state. (C) 2011 Elsevier Inc. All rights reserved.

DOI： 10.1016/j.jms.2011.04.003

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Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：CANADIAN SCIENCE PUBLISHING, NRC RESEARCH PRESS  

Additional high-resolution lines in the nu(3) CO2 fundamental band of the rovibrational spectrum of He-2-CO2 have been observed using a tunable infrared laser to probe a pulsed supersonic jet expansion. The ro-vibrational spectrum was calculated using Euler angles and five vibrational coordinates that specify the positions of the He atoms with respect to the CO2 molecule, a product basis, and a Lanczos eigensolver. Rotational states with J = 0, 1, 2, and 3 associated with the vibrational ground state and different states (nu(t)) of the torsional motion of the two He atoms about the CO2 axis are identified and assigned. The assignment is consistent with having different principle axis orientiations in nu(t) = 0 and nu(t) = 1 states. Delta nu(t) = 1 infrared transistions are forbidden due to the symmetry of CO2, but Delta nu(t) = 1 microwave transistions are possible. Theoretical line positions and intensities are predicted. Good agreement between experiment and theory was obtained. The calculated energy levels and intensities were crucial in assigning some of the weaker observed transitions.

DOI： 10.1139/P08-119

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Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

High-resolution infrared spectra of clusters containing para-H2 and/or ortho-H2 and a single nitrous oxide molecule are studied in the 2225-cm(-1) region of the upsilon1 fundamental band of N2O. The clusters are formed in pulsed supersonic jet expansions from a cooled nozzle and probed using a tunable infrared diode laser spectrometer. The simple symmetric rotor-type spectra generally show no resolved K structure, with prominent Q-branch features for ortho-H2 but not para-H2 clusters. The observed vibrational shifts and rotational constants are reported. There is no obvious indication of superfluid effects for para-H2 clusters up to N=13. Sharp transitions due to even larger clusters are observed, but no definite assignments are possible. Mixed (para-H2)N-(ortho-H2)M-N2O cluster line positions can be well predicted by linear interpolation between the corresponding transitions of the pure clusters.

PubMed

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Language：English   Publishing type：Research paper (scientific journal)  

Rovibrational spectra of the He(2)-N(2)O complex in the nu(1) fundamental band of N(2)O (2224 cm(-1)) have been observed using a tunable infrared laser to probe a pulsed supersonic jet expansion, and calculated using five coordinates that specify the positions of the He atoms with respect to the NNO molecule, a product basis, and a Lanczos eigensolver. Vibrational dynamics of the complex are dominated by the torsional motion of the two He atoms on a ring encircling the N(2)O molecule. The resulting torsional states could be readily identified, and they are relatively uncoupled to other He motions up to at least upsilon(t) = 7. Good agreement between experiment and theory was obtained with only one adjustable parameter, the band origin. The calculated results were crucial in assigning many weaker observed transitions because the effective rotational constants depend strongly on the torsional state. The observed spectra had effective temperatures around 0.7 K and involved transitions with J < or =3, with upsilon(t) = 0 and 1, and (with one possible exception) with Deltaupsilon(t)=0. Mixing of the torsion-rotation states is small but significant: some transitions with Deltaupsilon(t) not equal 0 were predicted to have appreciable intensity even assuming that the dipole transition moment coincides perfectly with the NNO axis. One such transition was tentatively assigned in the observed spectra, but confirmation will require further work.

PubMed

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Language：English   Publishing type：Research paper (scientific journal)  

The design and operation of an apparatus for studying infrared spectra of weakly-bound complexes is described in detail. A pulsed supersonic jet expansion is probed using a tunable Pb-salt diode laser spectrometer operated in a rapid-scan mode. The jet may be fitted with either pinhole or slit shaped nozzles, the former giving lower effective rotational temperatures, and the latter giving sharper spectral lines. Notable features of the apparatus include use of a toroidal multi-pass mirror system to give over 100 passes of the laser through the supersonic jet, use of the normal laser controller for laser sweeping during both setup and data acquisition, and use of a simple semi-automated wavenumber calibration procedure. Performance of the apparatus is illustrated with observed spectra of the van der Waals complex He-OCS, and the seeded helium clusters He(N)-OCS and He(N)-CO.

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Language：English   Publishing type：Research paper (scientific journal)  

Infrared spectra of He(N)-CO(2) clusters with N up to about 20 have been studied in the region of the CO(2) nu(3) fundamental band ( approximately 2350 cm(-1)) using a tunable diode laser spectrometer and pulsed supersonic jet source with cooled (>-150 degrees C) pinhole or slit nozzles and high backing pressures (<40 atm). Compared to previous studies of He(N)-OCS and -N(2)O clusters, the higher symmetry of CO(2) results in simpler spectra but less information content. Discrete rotation-vibration transitions have been assigned for N=3-17, and their analysis yields the variation of the vibrational band origin and B rotational constant over this size range. The band origin variation is similar to He(N)-OCS, with an initial blueshift up to N=5, followed by a monotonic redshift, consistent with a model where the first five He atoms fill a ring around the equator of the molecule, forcing subsequent He atom density to locate closer to the ends. The B value initially drops as expected for a normal molecule, reaching a minimum for N=5. Its subsequent rise for N=6 to 11 can be interpreted as the transition from a normal (though floppy) molecule to a quantum solvation regime, where the CO(2) molecule starts to rotate separately from the He atoms. For N>13, the B value becomes approximately constant with a value about 17% larger than that measured in much larger helium nanodroplets.

PubMed

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DOI： 10.1016/j.jms.2003.10.009

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DOI： 10.1063/1.1758701

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DOI： 10.1063/1.1774158

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Language：English   Publishing type：Research paper (scientific journal)  

High resolution microwave and infrared spectra of He(N)-N2O clusters were studied in the range N=3 to 12. The apparent cluster moments of inertia increase from N=3 to 6, but then decrease, showing oscillatory behavior for N=7 to 12. This provides direct experimental evidence for the decoupling of helium atoms from the rotation of the dopant molecule in this size regime, signaling the transition from a molecular complex to a quantum solvated system and directly exploring the microscopic evolution of "molecular superfluidity."

PubMed

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DOI： 10.1063/1.1598954

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DOI： 10.1063/1.1578473

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：AMER INST PHYSICS  

Infrared spectra of the weakly bound complexes N2O-He-4, N2O-He-3, and OCS-He-3 have been observed using a tunable diode laser to probe a pulsed supersonic jet expansion. The rotational structure of the bands was analyzed using a conventional asymmetric rotor Hamiltonian. The N2O-He-3 and OCS-He-3 spectra are mostly a type (DeltaK(a)=0) in structure, with very weak b-type (DeltaK(a)=+/-1) transitions, but for N2O-He-4 the a- and b-type components are both prominent. The fitted rotational parameters are consistent with roughly T-shaped structures with intermolecular separations around 3.4-3.5 Angstrom for N2O-He and 3.8-3.9 Angstrom for OCS-He. The angle between the N2O or OCS axis and the He position is about 80degrees for N2O-He and 65degrees for OCS-He. The vibrational band origins are slightly blueshifted from those of the free molecule, with the N2O-He shifts (+0.2 cm-1) being about twice the magnitude of the OCS-He shifts (+0.1 cm(-1)). The results are of particular interest since N2O and (especially) OCS have both been used as probes in experiments on ultracold helium nanodroplets. (C) 2002 American Institute of Physics.

DOI： 10.1063/1.1493191

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：ACADEMIC PRESS INC ELSEVIER SCIENCE  

The millimeter-wave spectrum of the normal isotope of the CO dimer, ((CO)-C-12-O-16)(2), has been systematically surveyed in the regions 75-105 and 131-174 GHz, with additional measurements covering the entire 60-176 GHz range. By combining these results and using the technique of combination differences based on previously known energy levels, 14 new rotational levels have been assigned and precisely (approximate to0.1 MHz) located. They belong to 3 completely new states, 1 with A(+) symmetry and 2 with A(-) symmetry. The position of the lowest energy A(-) state results in a new and lower value for the effective tunneling splitting of the CO dinner, 3.73 cm(-1). The observation of dramatically different intensities for different bands supports the concept of two isomeric forms for (CO)(2), the ground state having a larger intermolecular separation (approximate to4.4 Angstrom) with most likely a C-bonded configuration, and the low-lying 0,88 cm(-1)) excited state having a smaller separation (approximate to4.0 Angstrom) and an O-bonded geometry. (C) 2002 Elsevier Science (USA).

DOI： 10.1006/jmsp.2002.8579

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DOI： 10.1063/1.1413978

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DOI： 10.1063/1.1514207

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DOI： 10.1063/1.1386920

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DOI： 10.1006/jmsp.1999.7844

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DOI： 10.1016/s0009-2614(99)01213-0

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DOI： 10.1063/1.471652

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DOI： 10.1006/jmsp.1996.0174

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DOI： 10.1063/1.472715

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DOI： 10.1006/jmsp.1995.1008

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DOI： 10.1006/jmsp.1993.1253

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Event date： 2019.10.21

Language：Japanese   Presentation type：Oral presentation (invited, special)  

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Event date： 2019.9.17 - 2019.9.18

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Event date： 2019.3.26 - 2019.3.27

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Event date： 2017.5.19 - 2017.5.20

Event date： 2016.6.20 - 2016.6.24

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Venue：University of Illinois at Urbana-Champaign   Country：United States  

Event date： 2015.8

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