Abstract
In this paper, we present Monte Carlo simulations of helium droplet pick-up experiments with the intention of developing a robust and accurate theoretical approach for interpreting experimental helium droplet calorimetry data. Our approach is capable of capturing the evaporative behavior of helium droplets following dopant acquisition, allowing for a more realistic description of the pick-up process. Furthermore, we circumvent the traditional assumption of bulk helium behavior by utilizing density functional calculations of the size-dependent helium droplet chemical potential. The results of this new Monte Carlo technique are compared to commonly used Poisson pick-up statistics for simulations that reflect a broad range of experimental parameters. We conclude by offering an assessment of both of these theoretical approaches in the context of our observed results.
Highlights
Under ambient pressure and temperatures approaching absolute zero, helium transforms from its gaseous state into a superfluid by means of Bose-Einstein condensation.[1,2,3] This gives rise to many interesting quantum phenomena and, for spectroscopists, offers a unique cryogenic matrix with which to study embedded molecules and molecular clusters
Helium droplets are transparent to many kinds of radiation and interact with residing species only slightly, meaning they are less perturbing than other ultra-cold techniques
Helium droplets and their acquired dopants are probed via depletion studies, in which portions of the droplets are evaporated by energy released through chemical reactions of the dopant atom(s) or molecule(s), or by energy deposited in the droplet after the dopant absorbs a photon
Summary
Under ambient pressure and temperatures approaching absolute zero, helium transforms from its gaseous state into a superfluid by means of Bose-Einstein condensation.[1,2,3] This gives rise to many interesting quantum phenomena and, for spectroscopists, offers a unique cryogenic matrix (in the form of helium droplets) with which to study embedded molecules and molecular clusters. Helium droplets and their acquired dopants are probed via depletion studies, in which portions of the droplets are evaporated by energy released through chemical reactions of the dopant atom(s) or molecule(s), or by energy deposited in the droplet after the dopant absorbs a photon. By monitoring this change in droplet size, the amount of energy thereby deposited can be deduced.
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