Conservation of Hot Thermal Spin-Orbit Population of 2 P Atoms in a Cold Quantum Fluid Environment

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Abstract

The 0.4 K internal temperature of superfluid helium nanodroplets is believed to guarantee a corresponding ground-state population of dopant atoms and molecules inside this cryogenic matrix. We have recorded 6s ← 5p excitation spectra of indium atoms in helium droplets and found two absorption bands separated by about 2000 cm - 1 , a value close to the spin-orbit (SO) splitting of the In 2 P ground state. The intensities of the bands agree with a thermal population of the 2 P 1/2 and 2 P 3/2 states at 870 K, the temperature of the In pick-up cell. Applying femtosecond pump-probe spectroscopy, we found the same dynamical response of the helium solvation shell after the photoexcitation of the two bands. He-density functional theory simulations of the excitation spectra are in agreement with the bimodal structure. Our findings show that the population of SO levels of hot dopants is conserved after pick-up inside the superfluid droplet. Implications for the interpretation of experiments on molecular aggregates are discussed.

LanguageEnglish
Pages3977-3984
Number of pages8
JournalJournal of Physical Chemistry A
Volume123
Issue number18
DOIs
StatusPublished - 9 May 2019

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Helium
Ground state
conservation
Conservation
Orbits
helium
Doping (additives)
Superfluid helium
orbits
Atoms
Indium
Fluids
Photoexcitation
fluids
Solvation
Cryogenics
Density functional theory
atoms
Absorption spectra
ground state

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry

Cite this

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title = "Conservation of Hot Thermal Spin-Orbit Population of 2 P Atoms in a Cold Quantum Fluid Environment",
abstract = "The 0.4 K internal temperature of superfluid helium nanodroplets is believed to guarantee a corresponding ground-state population of dopant atoms and molecules inside this cryogenic matrix. We have recorded 6s ← 5p excitation spectra of indium atoms in helium droplets and found two absorption bands separated by about 2000 cm - 1 , a value close to the spin-orbit (SO) splitting of the In 2 P ground state. The intensities of the bands agree with a thermal population of the 2 P 1/2 and 2 P 3/2 states at 870 K, the temperature of the In pick-up cell. Applying femtosecond pump-probe spectroscopy, we found the same dynamical response of the helium solvation shell after the photoexcitation of the two bands. He-density functional theory simulations of the excitation spectra are in agreement with the bimodal structure. Our findings show that the population of SO levels of hot dopants is conserved after pick-up inside the superfluid droplet. Implications for the interpretation of experiments on molecular aggregates are discussed.",
author = "Bernhard Thaler and Ralf Meyer and Pascal Heim and Sascha Ranftl and Pototschnig, {Johann V.} and Hauser, {Andreas W.} and Markus Koch and Ernst, {Wolfgang E.}",
year = "2019",
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language = "English",
volume = "123",
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journal = "The journal of physical chemistry (Washington, DC) / A",
issn = "1089-5639",
publisher = "American Chemical Society",
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T1 - Conservation of Hot Thermal Spin-Orbit Population of 2 P Atoms in a Cold Quantum Fluid Environment

AU - Thaler, Bernhard

AU - Meyer, Ralf

AU - Heim, Pascal

AU - Ranftl, Sascha

AU - Pototschnig, Johann V.

AU - Hauser, Andreas W.

AU - Koch, Markus

AU - Ernst, Wolfgang E.

PY - 2019/5/9

Y1 - 2019/5/9

N2 - The 0.4 K internal temperature of superfluid helium nanodroplets is believed to guarantee a corresponding ground-state population of dopant atoms and molecules inside this cryogenic matrix. We have recorded 6s ← 5p excitation spectra of indium atoms in helium droplets and found two absorption bands separated by about 2000 cm - 1 , a value close to the spin-orbit (SO) splitting of the In 2 P ground state. The intensities of the bands agree with a thermal population of the 2 P 1/2 and 2 P 3/2 states at 870 K, the temperature of the In pick-up cell. Applying femtosecond pump-probe spectroscopy, we found the same dynamical response of the helium solvation shell after the photoexcitation of the two bands. He-density functional theory simulations of the excitation spectra are in agreement with the bimodal structure. Our findings show that the population of SO levels of hot dopants is conserved after pick-up inside the superfluid droplet. Implications for the interpretation of experiments on molecular aggregates are discussed.

AB - The 0.4 K internal temperature of superfluid helium nanodroplets is believed to guarantee a corresponding ground-state population of dopant atoms and molecules inside this cryogenic matrix. We have recorded 6s ← 5p excitation spectra of indium atoms in helium droplets and found two absorption bands separated by about 2000 cm - 1 , a value close to the spin-orbit (SO) splitting of the In 2 P ground state. The intensities of the bands agree with a thermal population of the 2 P 1/2 and 2 P 3/2 states at 870 K, the temperature of the In pick-up cell. Applying femtosecond pump-probe spectroscopy, we found the same dynamical response of the helium solvation shell after the photoexcitation of the two bands. He-density functional theory simulations of the excitation spectra are in agreement with the bimodal structure. Our findings show that the population of SO levels of hot dopants is conserved after pick-up inside the superfluid droplet. Implications for the interpretation of experiments on molecular aggregates are discussed.

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U2 - 10.1021/acs.jpca.9b02920

DO - 10.1021/acs.jpca.9b02920

M3 - Article

VL - 123

SP - 3977

EP - 3984

JO - The journal of physical chemistry (Washington, DC) / A

T2 - The journal of physical chemistry (Washington, DC) / A

JF - The journal of physical chemistry (Washington, DC) / A

SN - 1089-5639

IS - 18

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