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Phase-sensitive detection of persistent spectral holes using synchronous ultrasonic modulation spectroscopy

W. E. Moerner, Alan L. Huston

Published Jun 9, 1986• 0 citations
OpenAlex

Abstract

Persistent spectral hole-burning (PHB) of inhomogeneously broadened absorption lines in solids occurs when a homogeneous class of absorbing centers in resonance with a narrowband laser beam undergoes a photolnduced change in optical absorption that persists for times longer than any excited state lifetime. Persistent spectral holes for impurity centers in solids can provide important information about guest–light and guest–host interactions, such as dephasing, Zeeman and Stark splittings, and photochemical reaction mechanisms.

Related papers

Molecular electronics for frequency domain optical storage: Persistent spectral hole-burning - A review

W. E. Moerner

Persistent spectral hole-burning (PHB) is a phenomenon that allows an additional dimension, the frequency at which spectral holes are written, to be used to encode digital data. PHB can be used to store a large number of bits of information in the volume irradiated by a focused laser beam, leading to a possible future storage technology, frequency domain optical storage. A large number of photochemical and photophysical mechanisms have led to the production of spectral holes; a wealth of information has been learned about host-guest interactions, dephasing, and solid-state photochemistry at low temperatures. The general structure of a frequency domain optical store places a set of constraints on the engineering of such a system as well as on the materials used as recording media. The dynamics of the hole-burning process are crucial; for monophotonic mechanisms in particular, a set of stringent constraints can be derived that limit the applicability of this class of materials. Recent discoveries of two-color, photon-gated hole-burning offer special promise for nondestructive reading and improved performance.

•Mar 25, 1985•10 citations

Observation of persistent spectral hole–burning in semiconductor nanocrystals

Yasuaki Masumoto, Lev Zimin, Kazuhiko Naoe

So far, persistent spectral hole-burning (PSHB) phenomenon has been observed in a number of materials. They are molecules in glasses, crystals and polymers, color centers in alkali halide crystals, and rare earth and transition metal ions in glasses and crystals. They are molecular or ionic guests embedded in glass, crystal or polymer hosts. Basic requirements for the PSHB are summarized as follows: (1) The optical absorption of guests embedded in hosts must be broadened inhomogeneously. (2) There must exist more than one ground state configurations of the total system consisting of guests and hosts. (3) The relaxation among the ground states must be slower than the decay rate of any excited state. In fact, this set of requirements is satisfied in many kinds of molecular or ionic guests in hosts, such as glasses, crystals and polymers, at low temperatures. We can naturally understand that guests consisting of small number of atoms are greatly influenced by the surrounding hosts and that the energy levels of the guests are inhomogeneously broadened.

Spectral Hole-Burning and Related Spectroscopies: Science and Applications•Jan 1, 1994•0 citations

TWO-COLOR, PHOTON-GATED SPECTRAL HOLE-BURNING

W. E. Moerner, Manfred Gehrtz, Howard W. H. Lee +4 more

Persistent spectral hole-burning (PHB) has been proposed as the essential element of a frequency domain optical storage system1 in which the frequency at which a hole is burned in an inhomogeneously broadened absorption line at low temperatures serves as an additional dimension for the storage of digital information. Essentially all of the mechanisms studied until recently have been single-photon mechanisms, i.e., the photoionduced change leading to hole-burning (writing) for a given center occurs with a certain fixed probability after the absorption of one photon. Such linear, monophotonic processes suffer from the drawback that the act of detecting holes (reading) can also produce changes in the absorption line. Recent modeling studies of the generalized single-photon process2 have shown that thousands to tens of thousands of reads can be obtained from single-photon mechanisms only when the material possesses high quantum efficiency and low absorption cross section. These restrictive requirements do not apply for photon-gated hole-burning mechanisms, i.e., those mechanisms for which hole-burning occurs only in the presence of an additional “gating” light source, because for these mechanisms, reading is performed in the absence of the gating light and is therefore nondestructive.

Conference on Lasers and Electro-Optics•Jan 1, 1985•0 citations

Incoherent Light Read-Out of Spectral Holograms

Anne Débarre, J. Keller, J.-L. Le Gouët +1 more

It is known that one has investigated two types of approach to Persistent Spectral Hole Burning (PHB), and to potential application for optical data storage. In both methods, a structure is stored within the inhomogeneously broadened optical absorption line of the guest ions or molecules in a host matrix at low temperature.

Spectral Hole-Burning and Related Spectroscopies: Science and Applications•Jan 1, 1991•0 citations

Reading and Writing of Photochemical Holes Using GaAIAs Diode Lasers

Peter Pokrowsky, W. E. Moerner, F. Chu +1 more

Many investigations have been done on the field of frequency domain optical memories based on photochemical hole burning (PHB). This effect offers an extra dimension for the organization of an optical memory. At cryogenic temperatures several solid state materials such as aggregate color centers in alkali halide crystals exhibit inhomogeneously broadened absorption lines. In such an absorption line permanent narrow holes can be burnt by photochemical processes induced by exposure to intense laser radiation with a wavelength within the inhomogeneously broadened line.

Optical Data Storage•Jan 1, 1983•0 citations

Electric Field Effect on Accumulated Photon Echoes in Dye Doped Polymers

Hansruedi Gygax, Alexander Rebane, H. Schwoerer +1 more

Persistent spectral hole-burning (PSHB) is a versatile tool to study Stark effect in solids where impurity spectra is strongly inhomogeneously broadened. At liquid helium temperatures impurity homogeneous zero-phonon line widths are small (γhom~10–2-10–4cm–1) and narrow holes can be burnt in the inhomogeneous distribution by illumination with narrow band laser(Δνlaser < γhom) U1- Stark effect alters the shape of narrow spectral holes depending on the Stark shift (splitting) of impurity energy levels, orientation of the impurities, strength and orientation of the electric field, as well as on the properties of the matrix [2].

Spectral Hole-Burning and Related Spectroscopies: Science and Applications•Jan 1, 1992•0 citations
Persistent spectral hole-burning (PHB) of inhomogeneously broadened absorption lines in solids occurs when a homogeneous class of absorbing centers in resonance with a narrowband laser beam undergoes a photolnduced change in optical absorption that persists for times longer than any excited state lifetime. Persistent spectral holes for impurity centers in solids can provide important information about guest–light and guest–host interactions, such as dephasing, Zeeman and Stark splittings, and photochemical reaction mechanisms.
Persistent spectral hole-burning (PHB) is a phenomenon that allows an additional dimension, the frequency at which spectral holes are written, to be used to encode digital data. PHB can be used to store a large number of bits of information in the volume irradiated by a focused laser beam, leading to a possible future storage technology, frequency domain optical storage. A large number of photochemical and photophysical mechanisms have led to the production of spectral holes; a wealth of information has been learned about host-guest interactions, dephasing, and solid-state photochemistry at low temperatures. The general structure of a frequency domain optical store places a set of constraints on the engineering of such a system as well as on the materials used as recording media. The dynamics of the hole-burning process are crucial; for monophotonic mechanisms in particular, a set of stringent constraints can be derived that limit the applicability of this class of materials. Recent discoveries of two-color, photon-gated hole-burning offer special promise for nondestructive reading and improved performance.
So far, persistent spectral hole-burning (PSHB) phenomenon has been observed in a number of materials. They are molecules in glasses, crystals and polymers, color centers in alkali halide crystals, and rare earth and transition metal ions in glasses and crystals. They are molecular or ionic guests embedded in glass, crystal or polymer hosts. Basic requirements for the PSHB are summarized as follows: (1) The optical absorption of guests embedded in hosts must be broadened inhomogeneously. (2) There must exist more than one ground state configurations of the total system consisting of guests and hosts. (3) The relaxation among the ground states must be slower than the decay rate of any excited state. In fact, this set of requirements is satisfied in many kinds of molecular or ionic guests in hosts, such as glasses, crystals and polymers, at low temperatures. We can naturally understand that guests consisting of small number of atoms are greatly influenced by the surrounding hosts and that the energy levels of the guests are inhomogeneously broadened.
Persistent spectral hole-burning (PHB) has been proposed as the essential element of a frequency domain optical storage system1 in which the frequency at which a hole is burned in an inhomogeneously broadened absorption line at low temperatures serves as an additional dimension for the storage of digital information. Essentially all of the mechanisms studied until recently have been single-photon mechanisms, i.e., the photoionduced change leading to hole-burning (writing) for a given center occurs with a certain fixed probability after the absorption of one photon. Such linear, monophotonic processes suffer from the drawback that the act of detecting holes (reading) can also produce changes in the absorption line. Recent modeling studies of the generalized single-photon process2 have shown that thousands to tens of thousands of reads can be obtained from single-photon mechanisms only when the material possesses high quantum efficiency and low absorption cross section. These restrictive requirements do not apply for photon-gated hole-burning mechanisms, i.e., those mechanisms for which hole-burning occurs only in the presence of an additional “gating” light source, because for these mechanisms, reading is performed in the absence of the gating light and is therefore nondestructive.
Many investigations have been done on the field of frequency domain optical memories based on photochemical hole burning (PHB). This effect offers an extra dimension for the organization of an optical memory. At cryogenic temperatures several solid state materials such as aggregate color centers in alkali halide crystals exhibit inhomogeneously broadened absorption lines. In such an absorption line permanent narrow holes can be burnt by photochemical processes induced by exposure to intense laser radiation with a wavelength within the inhomogeneously broadened line.
Persistent spectral hole-burning (PSHB) is a versatile tool to study Stark effect in solids where impurity spectra is strongly inhomogeneously broadened. At liquid helium temperatures impurity homogeneous zero-phonon line widths are small (γhom~10–2-10–4cm–1) and narrow holes can be burnt in the inhomogeneous distribution by illumination with narrow band laser(Δνlaser < γhom) U1- Stark effect alters the shape of narrow spectral holes depending on the Stark shift (splitting) of impurity energy levels, orientation of the impurities, strength and orientation of the electric field, as well as on the properties of the matrix [2].