Why hyperpolarizabllities fall short of the fundamental quantum limits

Kakoli Tripathy; Javier Pérez Moreno; Mark G. Kuzyk; Benjamin J. Coe; Koen Clays; Anne Myers Kelley

doi:10.1063/1.1795672

Why hyperpolarizabllities fall short of the fundamental quantum limits

Kakoli Tripathy, Javier Pérez Moreno, Mark G. Kuzyk, Benjamin J. Coe, Koen Clays, Anne Myers Kelley

Research output: Contribution to journal › Article › peer-review

Abstract

Linear spectroscopy, Raman spectroscopy, theory, and measured values of hyperpolarizability, were used to study the cause of gap between the experimental results and the fundamental limits. It was found that there is an apparent limit to the first hyperpolarizability that is about 10 -3/2 times the quantum limit. This gap cannot be explained by a dilution effect due to the presence of vibronic states. The results show that this gap is due to an unfavorable arrangement of excited state energies.

Original language	English
Pages (from-to)	7932-7945
Number of pages	13
Journal	Journal of Chemical Physics
Volume	121
Issue number	16
DOIs	https://doi.org/10.1063/1.1795672
Publication status	Published - 22 Oct 2004

Keywords

UV and visible spectra (absorption; why hyperpolarizabilities fall short of fundamental quantum limits); Harmonic oscillator (clipped; why hyperpolarizabilities fall short of fundamental quantum limits); Quantum transition (dipole moment; why hyperpolarizabilities fall short of fundamental quantum limits); Electronic state; Energy level; Excited state; Optical hyperpolarizability; Sum rule; Vibrational frequency; Vibronic level (why hyperpolarizabilities fall short of fundamental quantum limits)

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title = "Why hyperpolarizabllities fall short of the fundamental quantum limits",

abstract = "Linear spectroscopy, Raman spectroscopy, theory, and measured values of hyperpolarizability, were used to study the cause of gap between the experimental results and the fundamental limits. It was found that there is an apparent limit to the first hyperpolarizability that is about 10 -3/2 times the quantum limit. This gap cannot be explained by a dilution effect due to the presence of vibronic states. The results show that this gap is due to an unfavorable arrangement of excited state energies.",

keywords = "UV and visible spectra (absorption; why hyperpolarizabilities fall short of fundamental quantum limits); Harmonic oscillator (clipped; why hyperpolarizabilities fall short of fundamental quantum limits); Quantum transition (dipole moment; why hyperpolarizabilities fall short of fundamental quantum limits); Electronic state; Energy level; Excited state; Optical hyperpolarizability; Sum rule; Vibrational frequency; Vibronic level (why hyperpolarizabilities fall short of fundamental quantum limits)",

author = "Kakoli Tripathy and Moreno, {Javier P{\'e}rez} and Kuzyk, {Mark G.} and Coe, {Benjamin J.} and Koen Clays and Kelley, {Anne Myers}",

year = "2004",

month = oct,

day = "22",

doi = "10.1063/1.1795672",

language = "English",

volume = "121",

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journal = "Journal of Chemical Physics",

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T1 - Why hyperpolarizabllities fall short of the fundamental quantum limits

AU - Tripathy, Kakoli

AU - Moreno, Javier Pérez

AU - Kuzyk, Mark G.

AU - Coe, Benjamin J.

AU - Clays, Koen

AU - Kelley, Anne Myers

PY - 2004/10/22

Y1 - 2004/10/22

N2 - Linear spectroscopy, Raman spectroscopy, theory, and measured values of hyperpolarizability, were used to study the cause of gap between the experimental results and the fundamental limits. It was found that there is an apparent limit to the first hyperpolarizability that is about 10 -3/2 times the quantum limit. This gap cannot be explained by a dilution effect due to the presence of vibronic states. The results show that this gap is due to an unfavorable arrangement of excited state energies.

AB - Linear spectroscopy, Raman spectroscopy, theory, and measured values of hyperpolarizability, were used to study the cause of gap between the experimental results and the fundamental limits. It was found that there is an apparent limit to the first hyperpolarizability that is about 10 -3/2 times the quantum limit. This gap cannot be explained by a dilution effect due to the presence of vibronic states. The results show that this gap is due to an unfavorable arrangement of excited state energies.

KW - UV and visible spectra (absorption; why hyperpolarizabilities fall short of fundamental quantum limits); Harmonic oscillator (clipped; why hyperpolarizabilities fall short of fundamental quantum limits); Quantum transition (dipole moment; why hyperpolariz

U2 - 10.1063/1.1795672

DO - 10.1063/1.1795672

M3 - Article

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SP - 7932

EP - 7945

JO - Journal of Chemical Physics

JF - Journal of Chemical Physics

IS - 16

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Why hyperpolarizabllities fall short of the fundamental quantum limits

Abstract

Keywords

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