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Laser-heating of a transparent crystal via adsorbed atoms

Sander van Smaalen, Henk F. Arnoldus, Thomas F. Atoms

Published Oct 1, 1986• 0 citations
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Abstract

A coated surface of a crystal is irradiated by intense infrared light. The optically active atomic bonds absorb photons from the laser field, and the subsequent spontaneous decay goes together with emissions of phonons into the crystal. This photon phonon conversion results in an energy flux into the crystal. An equation for this flux is derived from the master equation for the level populations of the dressed atomic states. The saturation limit is discussed, and the general theory is illustrated with two examples. Furthermore, it is outlined with qualitative arguments that quantum yield of photodesorption is not sensitive to the laser power. Keywords: Laser heating; Transparent crystal; VIA Adsorbed atoms; Photon phonon conversion; Master equation; photodesorption.

Related papers

Laser heating of a transparent crystal via adsorbed atoms

Sander van Smaalen, Henk F. Arnoldus, Thomas F. George

A coated surface of a crystal is irradiated by intense infrared light. The optically active atomic bonds absorb photons from the laser field, and the subsequent spontaneous decay goes together with emissions of phonons into the crystal. This photon-to-phonon conversion results in an energy flux into the crystal. An equation for this flux is derived from the master equation for the level populations of the dressed atomic states. The saturation limit is discussed, and the general theory is illustrated with two examples. Furthermore, it is outlined with qualitative arguments that the quantum yield of photodesorption is not sensitive to the laser power.

Physical review. B, Condensed matter•Jan 1, 1987•6 citations

Interaction of an adsorbed atom with a laser. Technical report

Henk F. Arnoldus, Sander van Smaalen, Thomas F. George

The irradiation by infrared laser light of an atom adsorbed on the surface of a harmonic crystal is considered. The dynamic coupling between the atom (its motion) and the substrate degrees of freedom (phonon field) in the presence of a confining potential well (van der Waals bond between atom and crystal) gives rise to thermal relaxation of this adbond configuration. Both the atom and the substrate are assumed to be transparent, but the bond is allowed to have non-vanishing dipole-moment matrix elements, which couple the external field to the adsorbate. The equation of motion for the reduced adbond density operator is obtained with reservoir theory, and the relaxation constants are expressed in properties of the crystal. With a similar method, the spectral profile for absorption of weak radiation is derived. Subsequently, the illumination by a strong finite-linewidth laser field which is in close resonance with a single transition of the adbond is examined. The optical Bloch equations in operator form are derived and applied to study the process of laser heating of the crystal. It is pointed out how this mechanism can be understood as resulting from (multi)photon-phonon conversion reactions which are mediated by the adbond.

•Dec 1, 1986•0 citations

Thermal relaxation of adsorbed atoms in an intense laser field

Henk F. Arnoldus, Sander van Smaalen, Thomas F. George

Adsorbed atoms on the surface of a harmonic lattice are immersed in a strong laser field. The optical Bloch equations are derived, which include the thermal relaxation and the coherent excitation of the adbond. This is accomplished by a transformation to dressed states, which diagonalizes the interaction with the laser. The single-phonon couplings are then understood as transitions between dressed states. The radiative contributions for arbitrarily strong fields are obtained in the master equation, and it is shown that the coherences with respect to the dressed states decay exponentially, due to the phonon relaxation. General properties of the competing phonon-induced redistribution and optical excitation of the level populations are presented, and exemplified by an explicit elaboration of a three-level system. The results are amenable to analytical evaluation once the interaction potential is prescribed, and extensions of the approach to include multiphonon processes are straightforward.

Physical review. B, Condensed matter•Nov 15, 1986•12 citations

Laser-linewidth effects on the photon–phonon conversion rate at a gas–solid interface

Henk F. Arnoldus, Thomas F. George

An atom, bounded to the surface of a crystal; absorbs photons from a strong incident laser field and subsequently emits phonons into the solid. In this paper we study the influence of the laser linewidth on this photon–phonon conversion process. The appearance of coherences obscures the interpretation of the equation of motion in terms of transition rates and prohibits the derivation of a master equation in the transient region. The absorbed energy from the driving field, which is assumed to be resonant with a set of two levels only, results from the work done by the external field on the transition dipole. In the steady state, the energy absorption from the radiation field equals the energy emission in the phonon field. It is shown that in this long-time limit the coherences can be expressed in terms of the populations, and hence the system is again described by a masterlike equation. Specific aspects of the finite laser bandwidth are pointed out.

Journal of the Optical Society of America B•Feb 1, 1987•3 citations

Theory of an infrared irradiated adbond

Sander van Smaalen, Thomas F. George

The dynamics of an adsorbed atom irradiated by an infrared laser in resonance with the vibrational levels of the adbond can be described by the reduced density matrix of the adbond. A nonperturbative approach for the laser-adbond interaction is presented. Relaxation against the substrate degrees of freedom is described by second-order perturbation theory. Both pulsed lasers and cw lasers are considered. Expressions for the transition probabilities are derived in the low-intensity and in the high-intensity limits. It appears that the time evolution of the occupation probabilities is coupled to those of the coherences, i.e., a master equation cannot be obtained. The time evolution of all the elements of the reduced density matrix has to be taken into account. These expressions act as a basis for the study of physical processes as resonant de sorption, resonant heating, and laser-induced thermal desorption. Resonant desorption is described by the addition of loss terms into the equations of motion of the occupation probabilities. Expressions for the rate of desorption as well as the rate of energy transfer to the substrate are given. In particular, a comparison is made for the effect of a cw laser vs a pulsed laser on the desorption and resonant heating.

International Laser Science Conference•Jan 1, 1986•0 citations

A quantum approach to cavity mediated laser cooling

Tony Blake

Cavity-mediated cooling has the potential to become one of the most efficient techniques to cool molecular species down to very low temperatures. This thesis studies the use of rate equations to analyse the cooling process in such systems. In particular the master equation is used to find rate equations that can determine the rate of change of phonons in the system. The general idea behind cavity cooling is the continuous conversion of phonons into cavity photons. While there is no spontaneous emission and decay rate associated with the concept of phonons, photons are created after a change in the phonon number has occurred and can then leak out through the cavity mirrors easily. Hence the conversion of phonons into photons can result in the constant removal of phonon energy from the system. In this thesis we compare cavity mediated cooling with single particle laser cooling. It is shown that cavity cooling is essentially the same as ordinary laser cooling. This is done by calculating the stationary state phonon number mss and the cooling rate y as a function of the system parameters. For example, when the trap phonon frequency υ is either much larger or much smaller than the cavity decay rate k , the minimum stationary state phonon number scales as k²/16v² (strong confinement regime) and as k/4 (weak confinement regime), respectively. Replacing k with Ѓ yields the steady states associated with ordinary laser cooling.

•Sep 1, 2011•0 citations
A coated surface of a crystal is irradiated by intense infrared light. The optically active atomic bonds absorb photons from the laser field, and the subsequent spontaneous decay goes together with emissions of phonons into the crystal. This photon phonon conversion results in an energy flux into the crystal. An equation for this flux is derived from the master equation for the level populations of the dressed atomic states. The saturation limit is discussed, and the general theory is illustrated with two examples. Furthermore, it is outlined with qualitative arguments that quantum yield of photodesorption is not sensitive to the laser power. Keywords: Laser heating; Transparent crystal; VIA Adsorbed atoms; Photon phonon conversion; Master equation; photodesorption.
A coated surface of a crystal is irradiated by intense infrared light. The optically active atomic bonds absorb photons from the laser field, and the subsequent spontaneous decay goes together with emissions of phonons into the crystal. This photon-to-phonon conversion results in an energy flux into the crystal. An equation for this flux is derived from the master equation for the level populations of the dressed atomic states. The saturation limit is discussed, and the general theory is illustrated with two examples. Furthermore, it is outlined with qualitative arguments that the quantum yield of photodesorption is not sensitive to the laser power.
The irradiation by infrared laser light of an atom adsorbed on the surface of a harmonic crystal is considered. The dynamic coupling between the atom (its motion) and the substrate degrees of freedom (phonon field) in the presence of a confining potential well (van der Waals bond between atom and crystal) gives rise to thermal relaxation of this adbond configuration. Both the atom and the substrate are assumed to be transparent, but the bond is allowed to have non-vanishing dipole-moment matrix elements, which couple the external field to the adsorbate. The equation of motion for the reduced adbond density operator is obtained with reservoir theory, and the relaxation constants are expressed in properties of the crystal. With a similar method, the spectral profile for absorption of weak radiation is derived. Subsequently, the illumination by a strong finite-linewidth laser field which is in close resonance with a single transition of the adbond is examined. The optical Bloch equations in operator form are derived and applied to study the process of laser heating of the crystal. It is pointed out how this mechanism can be understood as resulting from (multi)photon-phonon conversion reactions which are mediated by the adbond.
Adsorbed atoms on the surface of a harmonic lattice are immersed in a strong laser field. The optical Bloch equations are derived, which include the thermal relaxation and the coherent excitation of the adbond. This is accomplished by a transformation to dressed states, which diagonalizes the interaction with the laser. The single-phonon couplings are then understood as transitions between dressed states. The radiative contributions for arbitrarily strong fields are obtained in the master equation, and it is shown that the coherences with respect to the dressed states decay exponentially, due to the phonon relaxation. General properties of the competing phonon-induced redistribution and optical excitation of the level populations are presented, and exemplified by an explicit elaboration of a three-level system. The results are amenable to analytical evaluation once the interaction potential is prescribed, and extensions of the approach to include multiphonon processes are straightforward.
An atom, bounded to the surface of a crystal; absorbs photons from a strong incident laser field and subsequently emits phonons into the solid. In this paper we study the influence of the laser linewidth on this photon–phonon conversion process. The appearance of coherences obscures the interpretation of the equation of motion in terms of transition rates and prohibits the derivation of a master equation in the transient region. The absorbed energy from the driving field, which is assumed to be resonant with a set of two levels only, results from the work done by the external field on the transition dipole. In the steady state, the energy absorption from the radiation field equals the energy emission in the phonon field. It is shown that in this long-time limit the coherences can be expressed in terms of the populations, and hence the system is again described by a masterlike equation. Specific aspects of the finite laser bandwidth are pointed out.
The dynamics of an adsorbed atom irradiated by an infrared laser in resonance with the vibrational levels of the adbond can be described by the reduced density matrix of the adbond. A nonperturbative approach for the laser-adbond interaction is presented. Relaxation against the substrate degrees of freedom is described by second-order perturbation theory. Both pulsed lasers and cw lasers are considered. Expressions for the transition probabilities are derived in the low-intensity and in the high-intensity limits. It appears that the time evolution of the occupation probabilities is coupled to those of the coherences, i.e., a master equation cannot be obtained. The time evolution of all the elements of the reduced density matrix has to be taken into account. These expressions act as a basis for the study of physical processes as resonant de sorption, resonant heating, and laser-induced thermal desorption. Resonant desorption is described by the addition of loss terms into the equations of motion of the occupation probabilities. Expressions for the rate of desorption as well as the rate of energy transfer to the substrate are given. In particular, a comparison is made for the effect of a cw laser vs a pulsed laser on the desorption and resonant heating.
Cavity-mediated cooling has the potential to become one of the most efficient techniques to cool molecular species down to very low temperatures. This thesis studies the use of rate equations to analyse the cooling process in such systems. In particular the master equation is used to find rate equations that can determine the rate of change of phonons in the system. The general idea behind cavity cooling is the continuous conversion of phonons into cavity photons. While there is no spontaneous emission and decay rate associated with the concept of phonons, photons are created after a change in the phonon number has occurred and can then leak out through the cavity mirrors easily. Hence the conversion of phonons into photons can result in the constant removal of phonon energy from the system. In this thesis we compare cavity mediated cooling with single particle laser cooling. It is shown that cavity cooling is essentially the same as ordinary laser cooling. This is done by calculating the stationary state phonon number mss and the cooling rate y as a function of the system parameters. For example, when the trap phonon frequency υ is either much larger or much smaller than the cavity decay rate k , the minimum stationary state phonon number scales as k²/16v² (strong confinement regime) and as k/4 (weak confinement regime), respectively. Replacing k with Ѓ yields the steady states associated with ordinary laser cooling.